Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
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Nilofar Asim
,
Mohd Sukor Su’ait
Abstract
Graphene-based materials are widely applied due to their interesting physical and chemical properties, but their hydrophobic surface and toxicity to living creatures limit their application in some fields. Biopolymers are incorporated with graphene-based materials to overcome these issues and improve their biodegradability, biocompatibility, and ecological friendliness, and the synergetic effect enhances other properties as well. These properties make graphene-based materials a novel subject of interest in science and industry. In this study, the various applications of developed biopolymer/graphene-based composites are broadly addressed, and recent progress in the field is emphasized. Modification, stability, and compatibility are among the key merits for developing highly advanced composites with desirable properties. The major challenges and some recommendations in various applications based on reviewed studies are covered. However, the development of environmentally friendly, low-cost, high-quality, and large-scale biopolymer/graphene-based composites for specified applications is challenging. Studies based on application and trend are conducted. Opportunities and limitations can guide researchers in the field to solve challenges, provide directions for future studies, and optimize sustainable biopolymer/graphene-based composites for specified industrial applications.
Graphical abstract
1 Introduction
Since the discovery of graphene, its various derivatives are developed and extensively investigated for different applications. Graphene-based nanocomposites in different forms, such as films, 3D porous scaffolds, fibrils, hydrogel, and nacre-like structures, have been developed and studied [1,2].
Given the huge potential of utilizing waste materials as precursors for the preparation of graphene derivatives, the dependence of their morphology, structure, and properties on conversion methods and type and composition of waste materials should be considered [3,4].
The invention of graphene and its potential for making various composites have opened up new interesting research areas to tailor new materials with chemical and physical properties designed on the basis of their bonding mechanism [5]. Biopolymers are materials derived from biological sources, such as animals, microorganisms, and plants. Biopolymers, as potential materials to combine with graphene, have attracted huge attention because of their abundance, renewability, biodegradability, low cost, and various applications [5]. Figure 1 shows the various available biopolymers for combination with graphene-based materials.
![Figure 1
Classification of biopolymers (reprinted with permission from refs [5,6]).](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_001.jpg)
According to Rouf and Kokini [5], biopolymer–graphene composites are synthesized through (1) solution intercalation, (2) melt intercalation, and (3) in situ polymerization. Other methods such as wet spinning, electrospinning, freeze-drying, microwave synthesis, molecular beam epitaxy drop casting, and layer-by-layer assembly are also utilized by researchers to prepare biopolymer–graphene-based composites [6,7]. The preparation method has important influences on the prepared nanocomposites’ physical and chemical properties because of their effect on homogeneity (distribution), interaction, and structure [8]. Figure 2 depicts the various available interactions between graphene derivatives and biopolymers.
![Figure 2
Common enabling interactions between graphene-based materials and biopolymers (reproduced with permission from refs. [9,10]).](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_002.jpg)
Interfacial interactions, including covalent and noncovalent bonding, improve the mechanical properties of graphene-based nanocomposites. These different kinds of interactions usually work synergistically together, resulting in excellent integrated mechanical properties. Noncovalent bonding, including hydrogen bonding, ionic bonding, and π–π interactions, usually shows relatively weak strength compared with covalent bonding [10]. However, the mechanical properties of graphene-based nanocomposites have been enhanced via noncovalent bonding due to their easy construction with graphene nanosheets. Covalent bonding shows strong interfacial strength and can be tuned by adjusting the length of the molecule chain and the density of crosslinking. The use of small molecules as crosslinkers usually enhances strength and stiffness but results in relatively low toughness due to the restriction of sliding between adjacent graphene nanosheets. Recent investigations reveal that long-chain linear molecules are good for enhancing tensile strength and toughness. Compared with long-chain linear molecules, a polymer or macromolecules with active functional groups can achieve integrated strength, stiffness, and toughness due to their high density of covalent crosslinking [9]. Cellulose, the most abundant biopolymer on earth, is widely utilized for different applications. Despite the cheap and abundant resource for the preparation of cellulose from biomass, bacterial cellulose has attracted attention because the prepared cellulose does not attach to hemicellulose or lignin [11,12]. Bacterial cellulose can be utilized for various applications. Figure 3 shows the various preparation methods of graphene-based/bacterial cellulose nanocomposites.
![Figure 3
Some utilized processing routes for the preparation of bacterial cellulose–graphene oxide nanocomposites [11].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_003.jpg)
Some utilized processing routes for the preparation of bacterial cellulose–graphene oxide nanocomposites [11].
The flexible bacterial cellulose/graphene/polyaniline nanocomposite with excellent electrical conductivity is prepared via a facile two-step strategy and presents a high potential for application in electromagnetic shielding and flexible electrodes [13].
To overcome the utilization of the conventional chemical-based preparation method, Dhar et al. [14] prepared bacterial cellulose/graphene-based films via a single step in situ fermentation. The physicochemical and structural properties of the composite depend on reduced graphene oxide compositions and fermentation conditions. The excellent inherent properties of prepared composites suggest flexible electronic materials.
Luo et al. [15] developed a facile layer-by-layer assembly method to prepare bacterial cellulose/graphene oxide hydrogels with excellent mechanical properties. Hydrogels contain highly dispersed graphene oxide nanosheets bundled by 3D interconnected bacterial cellulose nanofibers. Considering that the properties of composites are highly related to the miscibility and compatibility of the components, their modification can improve their properties dramatically.
2 Physical and chemical modifications of biopolymer, graphene-based materials, and their composites
The graphene derivatives’ properties can be modified for different applications by tailoring their structural changes, activation, and functionalization. Modification methods include covalent functionalization, noncovalent functionalization, substitutional doping of graphene, and hybridization with nanoparticles and nanowires [16]. Noncovalent modification can use π–π interactions, van der Waals forces, ionic interactions, and hydrogen bonding [17].
Various available functional groups, such as carboxyl, amino, or hydroxyl groups, on the biopolymer can establish effective interactions with functional groups on graphene derivatives and prepare new environmentally friendly composites with wide applications, which depend on their composition, interaction, and preparation conditions [5,6].
Xiong et al. [9] investigated structures, morphologies, functionalization, and processing applications of various bionanocomposites. Synergy effects are due to the combination of biopolymers with other materials, and their interfacial interactions and structures control their properties in different applications. Preparation methods have vital effects on the nanocomposites’ properties.
The biopolymer can be modified by grafting, crosslinking, blending, and coating [18,19]. The physical modification with or without the destruction of granular structure can modify some biopolymer properties [20].
The combination of the hierarchical structures of biopolymer nanofibrils, such as cellulose, chitin, silk, and collagen nanofibrils, and the unique strength and toughness of graphene derivatives by a simple preparation method are opening a new interesting research field to prepare new modified nanocomposites for specified applications [21].
The functionalization of available groups on biopolymer can provide wide opportunities for the preparation of tailored graphene-based nanocomposites. Cellulose has three active hydroxyl groups, including the primary hydroxyl of C-6 and the secondary hydroxyls of C-2 and C-3, which can undergo a series of modification reactions (including esterification, etherification, crosslinking, and graft copolymerization) [22]. These reactions produce cellulose derivatives with functional groups, such as silylates, sulfates, sulfonates, amines, hemiacetals, azides, and carbanilates. These functionalized cellulose derivatives find applications in different fields, such as medicine, agriculture, or textile. Moreover, many applications of chitosan have been limited by its low solubility in the aqueous solution. The efficient transformations of chitin and chitosan have also been limited by the lack of organosolubility due to its high molecular weight and interunit hydrogen bonding [23]. The chemical modification of these biopolymers through the introduction of different protecting groups at the hydroxyl and amino groups enhances good bioactivity properties and increases the solubility in organic and aqueous media (physiological conditions). The main reactions are acylation, alkylation, quaternization, sulfation, azidation, and phosphonation. Figure 4 presents various functionalization methods for nanocellulose and chitin or chitosan.
![Figure 4
(a) General paths for the modification of nanocellulose (reproduced from refs. [24,25]). (b) Regioselective and chemoselective modifications of chitosan [26].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_004.jpg)
The addition of monosaccharides, disaccharides, and polysaccharides to graphene-based materials is considered a key modification approach for improving hydrophilicity and dispersibility in polar solvents and their biodegradability for biomedical and environmental applications [27]. Among the available various methods for the (poly)saccharide functionalization of graphene, click chemistry is considered one of the best methods [28]. Click chemistry is defined as numerous chemical reactions that have some important common characteristics, including high modularity, high chemical yield, no byproduct, and minimal sensitivity to oxygen, water, and solvent. Click chemistry enables the covalent attachment of functional groups with affinity to the π-conjugated surface of graphene. Accordingly, the modifications of graphene with polysaccharides either at its edges or at the basal plane become possible through different approaches. However, in some cases, other functionalization methods of graphene or graphene oxide are needed before click chemistry [27]. Therefore, various complementary methods to click chemistry that are typically performed on –COOH or –OH groups on the edge or epoxide groups on basal plane of graphene or graphene oxide are known. Oxygen-containing groups, including hydroxyl, carboxyl, and epoxy groups, on the surface of graphene oxide are used for common chemical reactions, such as esterification, isocyanation, carboxylic acylation, epoxy ring opening, diazotization, and addition [22]. The functionalization of carboxylic acid groups is performed through the addition of nucleophilic species, whereas the functionalization via epoxy groups is done through ring-opening reactions. Figure 5 presents other methods complementary to click chemistry. Li and Papadakis [27] reviewed various modifications of graphene-based materials with (poly)saccharides through click chemistry. Figure 6 presents the three types of polysaccharide/graphene modifications.
![Figure 5
Different methods for the functionalization of graphene (upper part) and graphene oxide (lower part) relevant/complementary to click chemistry (R1–R10, various substituents; Nu, nucleophile) [27].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_005.jpg)
Different methods for the functionalization of graphene (upper part) and graphene oxide (lower part) relevant/complementary to click chemistry (R1–R10, various substituents; Nu, nucleophile) [27].
![Figure 6
Schematic of the covalent functionalization of graphene via click chemistry in the (a) basal plane and (b) edges. (c) Noncovalent modification of graphene through π–π stacking interactions of a functionalized pyrene through click chemistry (L, linker; F, functional group attached through a click approach; R, random graphene substituent; ∟ and ◆, two complementary chemical parts prone to undergo click coupling) [27].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_006.jpg)
Schematic of the covalent functionalization of graphene via click chemistry in the (a) basal plane and (b) edges. (c) Noncovalent modification of graphene through π–π stacking interactions of a functionalized pyrene through click chemistry (L, linker; F, functional group attached through a click approach; R, random graphene substituent; ∟ and ◆, two complementary chemical parts prone to undergo click coupling) [27].
Functionalization and hybridization play important roles in dispersion, stabilization, reduction, and reinforcement of nanocellulose/graphene-based nanocomposites, which control their properties [29].
The interaction of graphene-based materials with biopolymers is due to available hydroxyl, epoxy, carbonyl, and carboxyl groups [30]. These interactions include covalent, electrostatic, hydrogen, and noncovalent bonds. Then, functionalization can modify graphene-based biopolymer composites for specified applications [6,31,32]. The main categories of graphene-based biopolymer composites include 3D porous scaffolds, electrospun mats, hydrogel, and nacre-like structures, which present different properties. However, preparation methods affect the properties of prepared composites [1].
The vacuum-assisted self-assembly method is used to prepare casein phosphopeptide-biofunctionalized graphene oxide nanoplatelets/cellulose nanofibers [33]. The prepared composites show high thermal conductivity and excellent flame retardancy.
The microstructure-tunable cellulose nanofiber/reduced graphene oxide aerogels developed via the concentration of cellulose nanofiber present lightweight and high-efficiency microwave absorption materials [34].
The functionalization of chitosan with sulfonated graphene oxide and polyvinyl alcohol results in polymer electrolyte membrane with remarkable increment in electrochemical properties for high-temperature energy applications [35,36].
3 Applications of biopolymer/graphene-based composites
Eco-friendly biopolymer/graphene-based composites with various physicochemical properties can be used for different applications. The following sections provide some references for other researchers utilizing biodegradable and biocompatible biopolymer/graphene-based composite materials for various applications, which sometimes overlap.
3.1 Application in the construction sector
The construction industry has a huge influence on the global economic growth. Finding construction materials with high performance, low cost, and sustainability is the center of concern for researchers in this field. The improvement of performance such as strength [37], barrier and permeability properties [38,39], leaching [40], and durability [41] by the addition of graphene-based materials to cement has been studied. Despite wide studies on utilizing biopolymers and graphene-based materials in cement, the addition of biopolymer/graphene-based composite materials into cement is rarely studied [42].
Thermal isolation materials are widely used to improve energy saving in industries and buildings [43]. Modified cellulose nanofiber/graphene oxide/sodium montmorillonite aerogel materials present improved properties compared with traditional organic insulation materials and are considered as potential materials in building insulation, firefighting, and the chemical industry [44]. Cao and Yuan [43] developed doped ammonium polyphosphate/graphene oxide/cellulose nanofiber-based aerogel with excellent thermal isolation and flame-retardant properties via the freeze-drying method. Composites prepared by utilizing expandable graphite/chemically treated pulverized oil palm empty fruit bunch fiber-reinforced epoxy exhibit improved fire resistivity, thermal properties, and mechanical properties [45].
Wicklein et al. [46] developed lightweight anisotropic foams on the basis of cellulose nanofibers, graphene oxide, and sepiolite nanorods through the freeze-casting of suspensions. The produced foams have excellent thermal-insulating and fire-retardant properties, which can be utilized in buildings. Spatial confinement and freeze-drying methods are used to prepare the hierarchical graphene-confined zirconium phosphate/cellulose nanofiber aerogel [47]. The prepared hybrid aerogel, which is mechanically stable and has outstanding thermal insulation and flame retardancy, can be utilized as a thermal insulator for improving energy efficiency in buildings. Guo et al. [48] prepared phosphorus-hybridized graphene nanosheets/cellulose nanofibers foam with excellent fire retardancy through the freeze-drying method.
Ternary nanocomposites utilizing bentonite, graphene oxide, and galactomannan crosslinked and strengthened with borate with the hierarchical structure are developed and exhibit high tensile stress and toughness. The brilliant fire-retardant property of these nanocomposites make them potential candidates in fire-protective insulation, packaging, and coating applications [49]. Efficient flame-retardant chitosan and graphene oxide in open-cell polyurethane foam coatings are prepared via layer-by-layer methods. The three bilayers exhibit 54% reduction in the peak of heat release rate, whereas six bilayers slow down the volatile release to low flammability limit [50].
Wang et al. [51] developed the multifunctional hybrid film through the reduction of graphene oxide nanosheets in the presence of montmorillonite nanoplatelets and cellulose nanofibers via vacuum filtration. The film has outstanding fire resistance, high thermal stability, and good flexibility. Its high dielectric constant and low dielectric loss show its potential as dielectric material in the capacitor field application.
Metal corrosion considers global challenges that seriously affect the economy, industry, and society [52]. Among various protection methods, anticorrosion coatings have attracted huge attention, and graphene-based anticorrosion coating materials are extensively studied [53,54,55]. However, chitosan, as a green, low-cost, and nontoxic natural biopolymer with good film-forming tendency, is used as anticorrosive coating for metals [56,57], and improved hydrophobicity by the incorporation of graphene-based materials leads to improved anticorrosion performance. Fayyad et al. [58] improved the anticorrosion performance of pure chitosan through the preparation of oleic acid-grafted chitosan/graphene oxide composite coating on carbon steel by 100-fold. The corrosion inhibition activities of some biopolymers as cheap, abundant, and eco-friendly counterpart in graphene-based composites have been studied to investigate the hybridizing effect. Graphene oxide–chitosan and graphene oxide–chitosan–ZnO composites have higher anticorrosion efficiencies by 83.8 and 85.6%, respectively, compared with graphene oxide [59]. The incorporation of modified gelatin and modified gelatin/graphene oxide in epoxy coating shows better anticorrosion performance on mild steel compared with pure epoxy coating [60]. Homogeneously dispersed graphene oxide improves the compactness and crosslinking degree of coating and increase the anticorrosion performance of coating by 59%. These results are promising for conducting research for the development of green and improved anticorrosion coating by incorporating biopolymer/graphene-based composites into usual coating materials. Linseed oil-based/reduced graphene oxide nanocomposites with anticorrosion properties exhibit the decreased corrosion rate by around 5,000 times when applied on mild steel [61].
Despite utilizing various phase-change materials in walls, floor heating, and building envelopes, which can consist of biopolymer/graphene-based composites for energy management in buildings, these composites will be reviewed under phase-change materials in the following subsections.
3.2 Biopolymer/graphene-based composites for catalyst applications
Despite developing various graphene-based composite for fuel cell application [62], biopolymer/graphene-based nanocomposites can be considered as green substrates for various catalyst materials. The synergetic effect of nanocomposite can promote the catalyst performance.
Pt/1,1′-dimethyl-4,4′-bipyridinium dichloride-functionalized graphene oxide/chitosan shows good catalytic activity for methanol [63] and ethanol electro-oxidation methods for direct ethanol fuel-cell application [64]. Pd-functionalized chitosan/reduced graphene oxide is developed as a catalyst with high activity and stability for formic acid electro-oxidation reaction in fuel cells [65].
The Pd/graphene oxide/chitosan/cellulose nanowhisker hydrogel presents good catalytic activity in the Mizoroki–Heck reaction to generate new C–C bonds [66].
Esmaeilzadeh et al. [67] synthesized Pd immobilized on the hybrid of magnetic graphene quantum dots/cyclodextrin-decorated chitosan as a hydrogenation catalyst. Chitosan/glutaraldehyde/reduced graphene oxide/Pd composite hydrogels are prepared via crosslinking and exhibit promising catalytic performance for the degradation of p-nitrophenol and o-nitroaniline. The developed hydrogels are considered as a potential catalyst for the reduction of organic pollutants in wastewater treatment [68]. The synthesis of porous Pd/chitosan/reduced graphene oxide microspheres via etching and freeze-drying methods leads to active and easily recyclable catalysts for Heck reactions [69]. Developed sodium alginate/sulfonated graphene oxide using blending and casting methods [70] exhibit good results to be considered as a potential alternative membrane in direct methanol fuel cell application.
3.3 Biopolymer/graphene-based composites in medical applications
Graphene may be used for various applications, like biosensing, bioimaging, and medical and electronic devices [71]. For biological applications, the high dispersibility and stability of applied nanomaterials in biological fluids are important and considered as shortcomings for graphene nanomaterials because of their intrinsic properties. The tendency of graphene nanomaterials for the adsorption of proteins that make them prone to internalization by macrophages and clearance from the body due to shortage of their half-life in the blood circulation is another consequence of utilizing graphene-based nanomaterials in biological applications. Other drawbacks are toxicity, low biocompatibility, and in vivo distribution profile, which may cause adverse side effects [32].
Different modification and functionalization methods of graphene via covalent or noncovalent mechanism have been studied to improve the various properties of graphene, such as biodegradability, biocompatibility, and safety [16,17]. Consequently, various biocomposites, which utilize carbohydrates (such as cellulose, chitin, alginate, and cyclodextrins), are prepared and investigated [32,72]. For example, antibacterial graphene-reinforced composite coatings based on chitosan, hydroxyapatite, and antibiotic gentamicin are fabricated for bone tissue engineering [73]. Dacrory [74] recently reported the antimicrobial activity of dialdehyde cellulose/graphene oxide film against COVID-19. Many applications based on using graphene and biomolecules require biomolecules (such as peptides, proteins, and enzymes) to interact with graphene at one end while simultaneously exposing the other end to the surrounding medium for biosensing analytes in solution. For example, the molecular interaction of graphene nanoribbons with peptides and enzymes present in the body for nanobiotechnological applications is reported [75]. Moreover, Wang and coworkers [76] successfully probed the molecular interaction of graphene oxide and nitrogen-functionalized graphene with bone morphogenetic protein-2 as key proteins implicated in bone repair with highest adsorption energy. Functionalization can provide different features for the development of an efficient drug delivery system with different drug release profiles, such as water solubility, biocompatibility, stability, bioavailability, and enhanced loading capacity, and reduce the immune system activation. Hybrid materials comprising graphene oxide, β-cyclodextrin, and poly(amidoamine) dendrimer are successfully prepared by covalent bonding and utilized as potential nanocarriers for anticancer drugs [77]. Moreover, Pooresmaeil et al. [78] utilized carboxymethyl cellulose as a coating agent for the encapsulation of magnetic graphene oxide coated with mesoporous silica for safe and sustained ibuprofen delivery. Shende and Pathan [72,79] extensively reviewed the interaction and application of various carbohydrate/graphene-based composites in biomedical fields, such as drug delivery and tissue engineering (Figures 7 and 8).
![Figure 7
Biomedical applications of carbohydrate–graphene-based nanocomposites [72,79].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_007.jpg)
![Figure 8
Methods for targeted delivery by graphene-based materials decorated with different carbohydrate polymers [32].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_008.jpg)
Methods for targeted delivery by graphene-based materials decorated with different carbohydrate polymers [32].
Functionalization can also provide the capability of targeting the nanocarrier, thereby improving the therapeutic efficiency (Figure 8). The modified graphene biocomposite tends to adsorb a wide range of hydrophobic drugs quickly and release them to the selected zone of organisms as a targeted drug delivery system. For example, galactosylated chitosan in combination with graphene oxide has been introduced as a new nanobiocomposite for doxorubicin delivery [80]. This strategy is considered advantageous because functionalized polymer–graphene biocomposites allow the targeting of high drug doses at the site of action, prevent the nonhomogenous biodistribution of therapeutic cargos, and overcome the adverse effects to the normal tissues caused by their interactions with anticancer therapeutics to an extent.
The biomedical application of graphene-based/biopolymer composites has been studied by Chen et al. [81]. Studies showed that graphene size and structure affect the properties of graphene–biopolymer composite properties [82,83]. Lalwani et al. [84] showed that the mechanical strength of biocomposite follows the order: graphene nanoplatelets > graphene nanoribbons > graphene nanotubes. These findings can extend their application in tissue engineering.
The antibacterial, antifungal, and antioxidant properties of graphene-based biopolymer composites make them interesting materials for active food packaging applications [85]. These properties are promoted because of the synergetic effect for free-radical inhibition (Figure 9). The amino and hydroxyl groups on biopolymers improve the oxidation inhibition by hydrogen donation [86].
![Figure 9
Improvement of the scavenger activity of reduced graphene oxide in the presence of free radicals when combined with natural bioactive compounds [86].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_009.jpg)
Improvement of the scavenger activity of reduced graphene oxide in the presence of free radicals when combined with natural bioactive compounds [86].
Preparation conditions, such as ultrasonication time and heat treatment, affect the properties of chitosan/graphene oxide nanocomposite films. Optimum conditions lead to the preparation of films with complete degradation property, which can be used as green packing materials, in soil compost within 28 days [87].
Sonication mixing and solution casting methods are used to prepare cellulose nanowhisker/graphene nanoplatelet films [88]. The prepared films show high thermal, electrical, and mechanical properties with potential as green antistatic and electronic packaging materials.
To overcome the low mechanical strength of hydrogel as a drawback in nerve tissue regeneration application, Jafarkhani et al. [89] developed nanographene oxide/chitosan hydrogels with a 20% increase in the nerve cell growth. The developed poly(vinyl alcohol)/chitosan/modified graphene oxide biocomposite presents improved antimicrobial and anti-inflammatory properties in vivo [90].
The design and preparation of graphene-based biomaterial scaffolds for neural regeneration application have been investigated by Reddy et al. [91]. Zhang et al. [92] synthesized antibacterial Ag-polydopamine/bacterial cellulose/reduced graphene oxide composite film, which shows excellent biocompatibility as wound dressing materials. Sodium alginate/graphene oxide/polyvinyl alcohol sponge nanocomposites prepared via the freeze–thaw cyclic process and freeze-dried molding show good water absorption, breathability, and mechanical properties. Investigation revealed that these nanocomposites are promising materials for wound healing applications. Despite the huge potential of chitosan as food packaging and wound healing materials, various modifications are required to tailor related properties, such as vapor permeability, optical transparency, and hydrophilicity. In this regard, the simple solvent casting method has been used to prepare flexible and transparent antimicrobial films by using chitosan/polyvinylpyrrolidone/graphene oxide nanosheets [93].
Bacterial cellulose/graphene-based composites show good potential in the biomedical application as well. Luo et al. [94] presented the improved cell behavior of graphene and graphene oxide in 3D nanofibrous bacterial cellulose scaffold compared with that of graphene. Rostami et al. [95] developed sharkskin-mimicked graphene oxide/chitosan membrane with improved antibacterial and cytocompatibility properties for diverse biomedical applications.
Qi et al. [96] prepared graphene oxide/poly-l-lysine composites films as bioscaffold coatings for potential application in stem cell research and developed a mild and inexpensive preparation method that can utilize other biomacromolecules, such as chitosan and gelatin in the composite preparation. The developed graphene nanoplatelet/hydroxyethyl cellulose graft poly(lactic acid) copolymer–polyurethane bionanocomposites with high thermal stability and water resistance show potential applications for electronics and medical areas [97].
Rebekah et al. [98] developed Fe nanoparticles decorated with graphene oxide/chitosan composite as a nanocarrier for protein delivery. The composite’s good drug loading and release profile make it a potential nanocarrier for clinical applications.
Functional 3D scaffold chitosan–graphite oxide nanoplatelet core–shell microparticles are synthesized via alkaline gelation and template-assisted assembly methods [99]. The outer shell protects the inner chitosan from enzymatic degradation and hydrophilic oxygen-containing functionalities on the outermost layer of graphene oxide, and its inner conductive graphitic core can maintain the bioactivity of the scaffold and promote the adhesion and growth of the neuronal cell.
3.4 Application as self-healing materials
Intelligent materials with the capability to respond to external stimulus, such as heat, electromagnetic wave, and mechanical force, and repair themselves after damage are self-healing materials. This ability allows them to refurbish their intrinsic properties and reach sustainable development by extending their lifetime, security, and saving cost [100]. Given their interesting graphene properties, self-healing graphene-based materials have attracted a huge interest. Considering the importance of preparation methods on the structure and properties of materials, various methods, such as solution mixing, in situ polymerization, layer-by-layer assembly, wet-fusing assembly, and hydrothermal method, are utilized to prepare graphene-based self-healing materials [100]. These materials can be utilized in different applications, such as biological applications, sensors [101], coatings [102,103], supercapacitors, flexible electronic devices and artificial skin, self-cleaning, adsorbent, biomimetic materials, and actuator. Figure 10 presents various forms of graphene-based self-healing composites. Graphene can be used as a reinforcement agent or a compound material in self-healing composites. The forms of graphene in self-healing materials are (a) graphene- [104], (b) graphene derivative- [105], and (c) crosslinked polymer/graphene-based [106] self-healing materials.
![Figure 10
Forms of graphene in self-healing materials: (a) graphene, (b) graphene derivatives, and (c) crosslinked polymer/graphene [100].](/document/doi/10.1515/ntrev-2022-0087/asset/graphic/j_ntrev-2022-0087_fig_010.jpg)
Forms of graphene in self-healing materials: (a) graphene, (b) graphene derivatives, and (c) crosslinked polymer/graphene [100].
The self-healing chitosan/graphene oxide nanosheet hydrogel prepared by the self-assembly method shows potential in biomaterial, wastewater treatment, and smart material applications [107].
Lee et al. [108] fabricated a series of self-healing composites by utilizing graphene-based biopolymers for advanced electromagnetic applications. The modified cellulose graphene-based nanocomposite reveals fast electronic self-healing property, making it an interesting candidate in self-healing electronics, artificial skins, soft robotics, biomimetic prostheses, and energy storage applications [109].
The crosslinking of hydrogel to achieve reversible coordination bonding is considered a method for the preparation of stimulus-responsive and self-healing materials. Wang et al. [110] prepared mussel-inspired catechol-containing polyaspartamide/graphene oxide hydrogel with highly improved storage, loss moduli, and tensile and compressive strengths as soft matter for biomedical applications. The photo-crosslinked gelatin/reduced graphene oxide hydrogel exhibits potential in rapid bone regeneration application [111].
Samadi et al. [112] developed polyvinyl alcohol/agar/graphene nanocomposite hydrogels based on three construct dynamic networks with high strength, toughness, and quick self-healing property for biomedical applications. The stretchable, self-healing, and conductive TEMPO-oxidized cellulose nanofiber/graphene nanocomposite hydrogel has been developed via an in situ free-radical polymerization with good potential in self-healing wearable electronics applications [113]. Xie et al. [114] developed the multifunctional flame-retardant nacre-inspired functional cellulose/graphene oxide nanocoating by using a one-step self-assembly method. Its ultrasensitive fire warning and self-healing make the nanocoating interesting materials in building, transportation, and electrical equipment applications.
Chitosan/graphene oxide composite hydrogels incorporated with mussel-inspired protein polydopamine have been developed [115]. Covalent bonds, supramolecular interactions, hydrogen bonding, and π–π stacking in these polydopamine-based hydrogels provide adhesive, conductive, self-healing, and fast-recovering hydrogels with remarkable potential in electroactive tissue engineering applications.
Three-dimensional bioprinted phenol-rich gelatin/graphene oxide hydrogel as a component for a myogenesis-inducing material is considered as potential materials in muscle tissue engineering and regenerative medicine application [116]. Bioderived aliphatic hyperbranched polyurethane/3-aminopropyltriethoxysilane-modified graphene oxide nanocomposites produce smart materials with considerable enhanced mechanical and self-healing properties under microwave and sunlight. These materials have versatile application as self-healing and self-cleaning materials [117].
Despite the preparation of the self-healing bio-based elastomer [118] and possibility of the addition of graphene-based materials, these composites have not been studied yet.
3.5 Application in electronics
The abundance, biocompatibility, biodegradability, lightweight, strong electrical conductivity, excellent ion conduction, and mechanical flexibility of biopolymers make them interesting materials for developing flexible, wearable, implantable, and environment-friendly electronic materials [119].
Given their functional groups, such as hydroxyl, amino, amine, and carboxylic groups, various molecular engineering strategies can be used to modify and tailor optoelectrical properties [120,121]. Their abundant functional groups provide high solubility and dispersion properties, thereby giving the potential to adopt low-temperature manufacturing methods and avoiding degradation caused by other tough techniques used for semiconductor patterning methods [119]. It provides an opportunity to develop low-cost, large-area, and flexible bioelectronic devices by using conventional printing techniques [119,122,123,124]. For example, the preparation of flexible nanofibrillated cellulose/reduced graphene oxide/carbon nanotube-conductive composite membrane via ultrasonic dispersion and low-temperature hot pressing leads to composite membranes with potential in conductive membranes, electrode materials, and other electronic applications [125].
The development of environmental-friendly triboelectric nanogenerator biopolymer/graphene-based composites can prepare potential low-cost and biocompatible materials for various applications [126]. Gao et al. [127] prepared a super-elastic, lightweight chitosan/graphene oxide scaffold with potential in mechanical cushioning, energy damping, and flexible device applications via bidirectional freezing and annealing.
3.6 Application in fuel cells
The request for low-cost polymers with optimized proton conductivity, reduced methanol crossover, and thermal stability for fuel-cell membrane is increasing [128]. Chitosan, as a cheap, abundant, and eco-friendly biodegradable polymer with amino/hydroxyl groups, is considered an interesting biopolymer to prepare biopolymer/graphene-based composites as proton-exchange membranes for fuel cell applications [129]. Various functionalization methods can be considered to overcome the low proton conductivity of chitosan. Shirdast et al. [130] prepared sulfonated chitosan/sulfonated graphene oxide membranes for fuel cell application. Nanocomposites showed high thermal/mechanical conductivity and selectivity (increases by 454 and 650%, respectively) properties compared with chitosan membranes for proton transport. Chen et al. [81] studied various preparation methods of advanced graphene-based/bio-based polymer composite membranes for fuel cell applications. Chitosan/sulfonated graphene oxide nanosheet membranes are developed as superior conduction proton-exchange membranes for fuel cells [131]. Pandy and Shahi [132] developed N,N-dimethylene phosphonic acid propylsilane graphene oxide/N-o-sulphonic acid benzyl chitosan with high water retention and conductivity for the preparation of multifunctional polymer electrolyte membranes.
Azli et al. [133] prepared potato starch/graphene oxide composite as the Li+ -conducting polymer electrolyte with high ionic conductivity and mechanical properties.
The layer-by-layer deposition method is used to prepare chitosan and graphene oxide on the membrane substrates of sulfonated poly(vinylidenefluoride) (PVdF) or sulfonated PVdF-co-hexafluoropropylene) for utilization as proton-exchange membrane in high-temperature fuel cells [134]. Yaqoob et al. [135] developed cellulose-derived graphene/polyaniline nanocomposites as novel and natural anode materials for benthic microbial fuel cells. The modified anode has higher performance by four times and high removal of Cd(ii) and Pb(ii) heavy metals from wastewater through benthic microbial fuel cells.
The synthesis of a new anion-exchange membrane with high conductivity achieves the utilization of cellulose, graphene oxide, and polyphenylene oxide [136]. After functionalization with 1,4-diazabicyclo [2.2.2] octane, the mechanically stable membrane shows a hydroxyl conductivity of 215 mS cm−1 at 80°C. Hosseinpour et al. [137] developed multilayer proton-exchange membrane utilizing cellulose nanocrystal for direct methanol fuel cell application. The developed membrane has presented a 20% increase in proton conductivity and 11% reduction in methanol crossover compared with Nafion N115.
3.7 Application in batteries
In the production of commercial Li-ion batteries as energy storage devices (including EV), active ingredient slurries are prepared using PVdF as a binder due to its adhesion properties and electrochemical stability. Unfortunately, some disadvantages, such as toxicity and nonenvironmental friendliness, are associated with the use of PVdF. N-Methyl-pyrrolidone (NMP) has been used as a solvent in the preparation of Li-ion electrodes, and both are costly [138,139,140]. The disadvantages of NMP are toxicity, nonvolatility (high melting point of about 200°C), and nonenvironmental friendliness because expensive solvents require high costs for purchase and waste maintenance [141]. Therefore, many researchers attempted to find other alternatives and investigate the suitability of other water-soluble, inexpensive, and environmental-friendly materials toward green binders to test as alternative binders (e.g., gelatin, chitosan tragacanth gum, and sodium alginate) [142]. Next, graphene can be considered as an active ingredient in preparing the biopolymer composite for Li-ion batteries due to its capability to participate in the energy storage intercalation mechanism (Figure 11). As reported by Raccichini et al. [143], an anode consisting of a single layer of graphene can host twice as many Li+ than that consisting of conventional graphite. The storage of a lithium ion on each side produces graphene in Li2C6 stoichiometry, which provides a specific capacity of 744 mA h g−1 that is twice that given by conventional graphite (372 mA h g−1) [144,145,146]. Sandwiched pyrolyzed bacterial cellulose/graphene oxide composite is prepared via a simple method [147]. Li–S batteries assembled with pure sulfur as cathodes and prepared composite interlayer exhibit around 600 mA h g−1 at 3 C and only 0.055% capacity decay per cycle, which can be observed in over 200 cycles.
Varieties of binders applied in electrode composition for Li-ion batteries.
Table 1 presents the data of some studies in biopolymer/graphene-based composites in batteries.
Studies related to biopolymer composite/Li and its specific capacities (mAh g−1)
| Ref. | Composites | Electrolytes | Properties |
|---|---|---|---|
| [148] | Graphite:graphene:CMC carrageenan | 1 M LiPF6, EC:EMC:DMC (1:1:1, v/v/v) | ▪Graphite:graphene vs roman in table 1:CMC carrageenan composite/Li achieves optimum discharge capacity and voltage range of 0.01–3.0 V. |
| ▪Q d = 202.2 mAh g−1 and CE of 94% for 100%:0%:10% composition | |||
| ▪Q d = 314.3 mAh g−1 and CE of 96% for 95%:5%:10% composition | |||
| ▪Q d = 304 mAh g−1 and CE of 93% for 90%:10%:10% composition | |||
| ▪Improved capacity, cycle performance, and CE effect of using CMC carrageenan binder over PVdF | |||
| ▪Increased CE effect of graphene addition | |||
| [148] | Graphite:graphene:CMC chitosan | 1 M LiPF6, EC:EMC:DMC (1:1:1, v/v/v) | ▪Graphite:graphene:CMC chitosan composite/Li achieves optimum discharge capacity and voltage range of 0.01–3.0 V. |
| ▪Q d = 324 mAh g−1 and CE of 93% for 100%:0%:10% composition | |||
| ▪Q d = 298 mAh g−1 and CE of 95% for 95%:5%:10% composition | |||
| ▪Q d = 386 mAh g−1 and CE of 91% for 90%:10%:10% composition | |||
| ▪Improved capacity, cycle performance, and CE effect of using CMC chitosan binder over PVdF | |||
| Pyrolyzed bacterial cellulose/graphene oxide | 1 mol LiTFSI and 4 wt% LiNO3 dissolved in (TEGDME) | ▪Sandwiched pyrolyzed bacterial cellulose/graphene oxide composite was prepared via a simple method. Li–S batteries were assembled with pure sulfur as cathodes, and the prepared composite interlayer exhibited around 600 mAh g−1 at 3 C and only 0.055% capacity decay per cycle, which could be observed in over 200 cycles | |
| [149] | (Si:graphite:graphene)/CB:biobinder BTR Co. Ltd, Shenzhen, China | 1 M LiPF6, EC:EMC:DMC (1:1:1, v/v/v) | ▪2%:8%:5% composition of Si:Graphite:Graphene/Li achieves optimum discharge capacity and voltage range of 0.01–2.0 V. |
| ▪Q d = 820.7 mAh g−1 and CE of 77.98% for 8%:1%:20% composition of (Si:graphite:graphene)/CB:BTR | |||
| ▪Superior cycle performance improvement effect of graphene addition | |||
| ▪Impedance reduction due to addition of graphene | |||
| [148] | Sn:PVDF/LiSn:CMC/LiSn:CMC:AB/Li | 1 M LiClO4, EC:DEC (1:1, v/v) | ▪Sn:PVDF/Li achieves optimum discharge capacity, voltage range of 0.01–2.0 V vs Li/Li+, Q d = 500 mAh g−1, and CE of 67.2% for 80%:20% composition. |
| ▪Sn:CMC/Li achieves optimum discharge capacity, voltage range of 0.01–2.0 V vs Li/Li+, Q d = 800 mAh g−1, and CE of 65.4% for 80%:20% composition. | |||
| ▪Sn:CMC:AB/Li achieves optimum discharge capacity, voltage range of 0.01–2.0 V vs Li/Li+, Q d = 800 mAh g−1, and CE of 76% for 60%:20%:20% composition. | |||
| ▪Superior cycle performance improvement of CMC binder effect | |||
| ▪The type of binder affects the capacitance performance of the LIB electrode | |||
| [150] | Graphite:graphene oxide:CB/Li | 1 M LiPF6, EC:DMC:DEC (1:1:1, v/v/v) | ▪Graphite:graphene oxide:CB/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V vs Li/Li+, and Q d = 450 mAh g−1 for GCG (75%:17%:8%) |
| ▪Graphite:graphene oxide:CB/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V Li/Li+, and Q d = 695 mAh g−1 for GCG (66%:17%:17%). | |||
| ▪Graphite:graphene oxide:CB/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V Li/Li+, and Q d = 590 mAh g−1 for GCG (58%:17%:25%). | |||
| ▪Graphene oxide serves as lithium storage and binder. | |||
| ▪Mixtures of carbon-based active materials can be blended into composites and affect the performance of LIB electrode capacitance | |||
| [140] | Graphite:SP:PVdF/LiGraphite:chitosan/Li | 1 M LiPF6, EC:DEC (1:1, v/v) | ▪Graphite:SP:PVdF/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V, Q d = 364.9 mAh g−1, and CE of 89.3% for 88.8%:3.2%:8% composition |
| ▪Graphite:chitosan/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V vs Li/Li+, Q d = 374 mAh g−1, and CE of 95.4% for 94%:6% composition. | |||
| ▪Improved capacity, cycle performance, and CE effect of the use of chitosan binders compared with those of PVdF | |||
| ▪Impedance reduction due to addition of graphene | |||
| [139] | Si:CB:PVdF/LiSi:CB:CMC chitosan Si:CB:alginate(62:30:8) at % composition | 1 M LiPF6, EC:DEC:DMC (1:1:1, v/v/v) 1 M LiPF6 | ▪Si:CB:PVdF/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V, Q d = 3579 mAh g−1, and CE of 71% |
| ▪Si:CB:CMC chitosan/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V, Q d = 4270 mAh g−1, and CE of 89% | |||
| ▪Si:CB:alginate/Li achieves optimum discharge capacity, voltage range of 0.01–3.0 V, Q d = 3807 mAh g−1, and CE of 86% | |||
| ▪Improved capacity, cycle performance, and CE effect of use of CMC chitosan binder over those of PVdF | |||
| ▪CMC chitosan serves as an effective binder for the Si anode |
3.8 Applications in supercapacitors
Supercapacitors with energy storage properties have fast charge–discharge process and outstanding cyclability and are considered environmentally friendly materials. Their performance depends on their surface area. Flexible supercapacitors require electrodes with high electrochemical performance and flexibility. The physical and chemical properties of nanocellulose and graphene-based materials make them interesting materials in supercapacitor application. Cellulose, as one of the most abundant natural organic polymers that originate from plants, woods, and bacteria, is a promising biopolymer with excellent mechanical properties, which can be improved by functionalization or structural modification [151].
Cellulose and its composites with various materials, such as lignin [152], have been used as electrodes, electrolytes, and membranes in supercapacitors [153,154]. Cellulose and its composites with different structures and properties can be utilized [21]. Graphene and graphene-based materials in various structures have been utilized extensively in supercapacitor application [155].
The use of nitrogen self-doped biopolymers, such as chitosan, in the preparation of graphene-based composite aerogels for high-performance supercapacitors also open new interesting research areas for the use of biopolymers in supercapacitors [156]. Various technologies, such as carbonization, biotemplate methods, and biocomplex technologies, can be used to prepare biopolymer-based composites for supercapacitors and other applications [157,158].
Xing et al. [159] reviewed the utilized design and preparation methods for nanocellulose/graphene-based composites in flexible supercapacitor application. Xing et al. [159] found out that controlling the distribution, structure, morphology, and quantity of nanoparticles on the surface; improving synergy in the composite; and simplifying the preparation process are the key factors for tailoring the properties of nanocellulose/graphene-based composites and their industrialization.
Liu et al. [160] developed 3D hierarchical porous glucose/graphene-based aerogels via hydrothermal and CO2 activation processes for gas adsorption and supercapacitor applications. Table 2 presents some studies conducted on biopolymer/graphene-based composites for supercapacitor application.
Selected studies on biopolymer/graphene-based composites in supercapacitors
| Composite | Property | Ref. |
|---|---|---|
| Fe3O4 nanoparticles embedded in cellulose nanofiber/graphite carbon hybrid aerogels | Capacitance and energy density of 5.82 F cm−3 and 2.35 mW h cm−3, respectively, and 94.7% of initial capacitance after 5,000 charge–discharge cycles | [161] |
| Flexible reduced graphene oxide/tin dioxide nanocomposite and cellulose fiber membranes | Capacitance of 53 F s−1 and 90% retention of its initial specific capacitance after 1,000 cycles | [162] |
| Carbonized cellulose nanofibril/graphene oxide composite aerogels | Capacitance of 398.47 F g−1 at the current density of 0.5 A g−1 and initial capacity maintained at 99.77% after 10,000 charge–discharge cycles | [163] |
| Cellulose/graphene oxide/polyaniline aerogel | Capacitance of 1218 mF cm−2 at the current density of 1.0 mA cm−2 and energy density of 258.2 µW h cm−2 at a power density of 1201.4 µW cm2 | [164] |
| Cellulose nanofibers/reduced graphene oxide/polypyrrole aerogel | Capacitance of 720 mF cm−2 at 0.25 mA cm–2 and 95% retention after 2,000 cycles | [165] |
| Cellulose/reduced graphene oxide/silver/Fe2O3 hybrid film | Capacitance of 2,044 mF cm−2 and areal energy density of 226.4 μW h cm−2 | [166] |
| 3D porous tannic acid/graphene-based composite by introducing Ni2+, Cu2+, and Fe3+ | Specific capacitance values of 373.6, 412.4, 460.4, and 429.4 F g−1 at 1 A g−1 and energy densities of 14.76, 16.76, 19.13, and 17.6 Wh kg−1 at 300 W kg−1 | [167] |
| Cellulose nanofibril/reduced graphene oxide/molybdenum oxynitride aerogel | Specific capacitance of 680 F g−1 in an aqueous electrolyte, 518 F g−1 in an ionic liquid electrolyte, and energy density of 114 Wh kg−1 | [168] |
| 3D nanocellulose/graphene/MnO2 composite | Capacitance of 212.73 F g−1 at 5 mV s−1 and stability of 86.5% capacitance retention ratio after 5,000 cycles at 2 A g−1 | [169] |
| Polypyrrole@TEMPO-oxidized bacterial cellulose/reduced graphene oxide macrofibers | Capacitance of 391 F g−1 at 0.5 A g−1 and energy density of 8.8 mW h cm−3 | [170] |
| 3D graphene oxide/bacterial cellulose fibers | Capacitance of 160 F g−1 at 0.4 A g−1 and capacitance retention of 90.3% over 2000 recycles | [171] |
| Nitrogen-doped MnO2 nanowire-reduced graphene oxide–cellulose nanofibril aerogel electrodes | Capacitance of 455.8 F g−1 and energy densities of 49.0 and 43.7 Wh kg−1 at power densities of 953.7 (aqueous electrolyte) and 948.3 (solid-state polymer gel electrolyte) W kg−1, respectively | [172] |
| Core–shell structured cellulose nanofibers/graphene@polypyrrole microfibers | Electrochemical properties (647 mF cm−2 and 14.37 µW h cm−2 at 0.1 mA cm−2), prominent cycling stability (92.5% capacitance retention and 92.6% coulomb efficiency after 10,000 cycles), and extraordinary flexibility (no significant decay in capacitance after 5,000 bending cycles) | [173] |
| 3D polypyrrole/bacterial cellulose/graphene composites | Highest electrical conductivity (1,320 S m−1) and volumetric capacitance (278 F cm−3) and 93.5% retention over 2,000 recycles | [174] |
| Graphene/silk fibroin-based carbon | Specific capacitance of 256 F g−1 at a current density of 0.5 A g−1 and 96.3% retention for 10,000 cycles at 5 A g−1 | [175] |
| 3D holey graphene oxide/bacterial cellulose | Specific capacity of 65.9 F g−1 at a current density of 0.4 A g−1 and an energy density of 9.2 Wh kg−1 at a power density of 112.9 W kg−1 | [176] |
3.9 Biopolymer/graphene-based composites as phase-change materials
Phase-change materials are promising for energy storage in smart thermal energy management, transfer, conversion (such as solar-to-thermal and electric-to-thermal), portable thermal energy, and advanced multifunctional areas [177]. Phase-change materials with low thermal conductivity can be utilized as a thermal insulator for buildings to maintain indoor thermal comfort and HVAC systems overload [178,179,180,181,182]. However, on the basis of their application overcoming their deficiencies, such as low thermal conductivity, low electrical conductivity, weak photo absorption, and shape instability, their performance should be increased. The incorporation of various carbon-based support materials, such as graphene-based nanostructure composites, is considered a versatile solution for these issues [177,183]. The modification can be done using various methods, such as physical blending, microencapsulation, spinning, and preconstruction 3D filler network [184].
Fatty acid/graphene and fatty acid/graphene oxide nanocomposites are promising materials for phase-change materials with high thermal conductivity [185]. Yuan et al. [186] prepared microcapsules of paraffin@ethylcellulose/methylcellulose/graphene oxide composite with improved photo-to-thermal conversion performance for solar–thermal storage application. The polyethylene glycol/cellulose/graphene aerogel is prepared via vacuum impregnation with high thermal conductivity, good shape stability, and large latent heat of fusion [187]. The incorporation of cellulose nanocrystals with graphene nanoplatelets and polyethylene glycol (PEG) control the leakage during phase transition and improve thermal conductivity [188]. The prepared composite has excellent light–thermal and electrothermal conversion capabilities. Thus, phase-change materials may provide stable temperature conditions for electronics operating in extreme environmental conditions. The new organic phase-change materials with a three-dimensional network are prepared by utilizing graphene nanoplatelet aerogel, melamine foam, cellulose nanofiber, and paraffin wax [189,190,191]. The developed phase-change material shows a 407% increase in thermal conductivity compared with paraffin wax and presents outstanding light–thermal and electrothermal transition capabilities. Considering the biomass waste management concept, the 3D, porous, reduced graphene oxide/modified spent coffee grounds with capability to adsorb 60% PEG is prepared and exhibits high leakage control performance [192]. The synthesized composite with high stability shows the excellent light–heat conversion rate, making the composite a good candidate for solar thermal storage in a short time.
Darzi et al. [193] prepared phase-change materials via the electrospinning of fatty acid ternary eutectic mixture with carbon fiber powder and graphene. The prepared nanofiber composites show improved thermal and electrical properties and potential for use in energy storage/retrieval systems operated in near-ambient temperatures. The performance improvement of paraffin as phase-change materials with multiwalled carbon nanotubes (MWCNT)-, graphene-, and MWCNT/graphene-based composites has been investigated [194]. Optimum composites show improved thermal conductivity and restrain the rapid rise in temperature of liquid phase-change composites and can be potential materials for lithium-ion power battery. The comb-like poly(hexadecyl acrylate) polymer is modified by its grafting to cellulose and modified graphene to increase its thermally induced flexibility for solar–thermal energy management [195]. The developed phase-change materials show high enthalpy, thermal conductivity, and physical strength. Oh et al. [196] prepared sodium sulfate decahydrate/nanofibril cellulose/graphite composite as phase-change materials with enhanced thermal conductivity by 250% for thermal energy storage application. Improved hydrogen bonding among fibrils and water molecules is the reason for thermal stability enhancement.
3.10 Application as sensor materials
The presence of various pollutant materials in air and water and the hazardous effects of creatures reveal the importance of sensors for their detection. Various fluorescence sensors for molecular recognition have been developed using functional nucleic acid-based composites due to their high flexibility [197]. Gao et al. [198] studied graphene-based DNA sensors. Lopez and Liu [199] reviewed the covalent and noncovalent functionalization of graphene oxide/DNA sensors. The advantages and disadvantages of each sensor are discussed.
Nanocellulose/graphene-based nanocomposites with outstanding mechanical properties and high electrical and thermal conductivity properties may be used in multisensing applications. These nanocomposites can respond to multiple stimuli, such as mechanical stimuli, environmental stimuli, and other human biosignals [29]. These nanocomposites can be combined with other materials to fabricate sensors. Various studies in this area are conducted and reviewed [29].
In biopolymer/graphene-based composite preparation, the homogenic dispersion of graphene-based materials in the polymer matrix is an important factor for the modification of its properties for various applications. Utilizing a facile, rapid, green, and inexpensive way for the large-scale preparation methods is important for commercialization and sustainability. Magerusan et al. [200] utilized the electrochemical exfoliation of graphite rods without the use of any organic solvent to prepare chitosan/graphene nanomaterial as a sunset yellow sensor. Table 3 lists some related studies in the sensor field.
Some biopolymer/graphene-based composites for sensor applications
| Composite | Detection | Ref. |
|---|---|---|
| Graphene oxide and G-quadruplex DNA | Ag+ and cysteine | [201] |
| Graphene oxide–DNA nanosystem | Live cell imaging and detection | [202] |
| DNA-grafted graphene oxide | pH biosensors | [203] |
| Graphene oxide/G-rich single-stranded DNA | K+ | [204] |
| Graphene oxide–quadruplex DNA | Pb2+ | [205] |
| Graphene oxide–DNAzyme | Pb2+ and Hg2+ | [206] |
| Cellulose/graphene-based nanocomposite | Multiple sensing (temperature, humidity, stress/strain, and liquids) | [207] |
| Cellulose/graphene nanoplate nanocomposite | Stretch and compress sensor | [208] |
| Cellulose nanofibers/graphene oxide composite | Humidity sensor and moist-induced electricity generator | [209] |
| Cellulose/reduced graphene oxide | Chemical vapor sensors | [210] |
| Cellulose paper coated with graphene | Humidity and piezoresistive force sensor | [211] |
| Cellulose/graphene/polyamide electrospun nanofibers | Hg2+ sensor | [212] |
| Bacterial cellulose/graphene oxide composite | Nitrite sensor | [213] |
| 3D bacterial cellulose/nitrogen-doped graphene oxide quantum dot | Iron ion sensor | [214] |
| Graphene/nafion/Pt NPs/chitosan/glucose oxidase | Glucose biosensor | [215] |
| Piezoresistive graphene–nanocellulose nanopaper | Strain sensor | [216] |
| Cellulose microfiber/reduced graphene oxide nanocomposite | Nitrobenzene sensor | [217] |
| Graphene/sodium alginate aerogels | Strain sensor | [218] |
| Reduced graphene oxide/cellulose films | Flexible temperature sensor | [219] |
3.11 Application in microextraction
Sample preparation in analytical chemistry is considered as the most time-consuming step and the main source of laboratory wastes. Microextraction methods with green solvents and sorbents are the solution to these issues. Biopolymers prove their potential as sorbents in microextraction methods due to their biodegradability, versatility, and easy functionalization [220]. Biopolymer/graphene-based composites also show promising performance as sorbent materials in microextraction. Table 4 presents samples for this application.
Some conducted studies on biopolymer/graphene-based composites in microextraction
| Composite | Application | Ref. |
|---|---|---|
| Graphene oxide/chitosan | Analysis of sulfonamide residues in egg and honey in liquid chromatography–ultraviolet detection | [221] |
| Hierarchically porous monolith polypyrrole/octadecyl silica/graphene oxide/chitosan cryogel | Extraction and preconcentration of carbamate pesticides in fruit juices | [222] |
| Hierarchical mercapto-grafted graphene oxide/magnetic chitosan | Preconcentration and extraction of mercury ion from water samples | [223] |
| Magnetic chitosan and graphene oxide functional guanidinium ionic liquid composite | Solid-phase extraction of protein | [224] |
| Graphene oxide–alizarin yellow R–magnetic chitosan nanocomposite | Selective determination of aluminum in water samples | [225] |
| Magnetic chitosan–Schiff base grafted on graphene oxide nanocomposite | Extraction and quantification of lead ion in blood samples | [226] |
| Molecular imprinted magnetic chitosan/graphene oxide | Selective separation/preconcentration of fluoxetine from environmental and biological samples | [227] |
| Magnetic graphene/chitosan nanocomposite | Nanoadsorbent for the removal of 2-naphthol from aqueous solution | [228] |
| Zn(ii)-imprinted polymer grafted on graphene oxide/magnetic chitosan nanocomposite | Extraction of zinc ions from different food samples | [229] |
| Magnetic chitosan/graphene oxide composite | Solid-phase extraction of phenyl urea herbicides | [230] |
| Magnetic graphene oxide/grafted chitosan copolymer | Adsorbent for catechin in magnetic solid-phase extraction | [231] |
| 3D Chitosan/reduced graphene oxide composites | Solid-phase extraction adsorbents for pesticide analysis | [232] |
| Alginate/graphene oxide biocomposite | Microsolid-phase extraction for nonsteroidal anti-inflammatory drugs | [233] |
3.12 Biopolymer/graphene-based composites for CO2 capture
The dramatic increase in atmospheric CO2 as greenhouse gas due to rapid industrialization and its effect on climate change make it an environmental concern in recent years. CO2 capture is considered a vital solution to overcome this issue [234]. Developing various materials for effective CO2 capture is an interesting research area. Various adsorbents are investigated for improved performance. Various materials, such as carbonaceous materials [234,235], nanoadsorbents [236], and inorganic-based materials [237,238], can be utilized in CO2 capture. Amine-rich solid sorbent materials are extensively studied for CO2 capture application [239]. Porous materials, such as aerogel, are considered as potential adsorbent materials for various applications, such as CO2 capture [240]. Chitosan, a low-cost, eco-friendly, and abundant natural polymer with amine groups, is considered an attractive material in CO2 capture application. However, the mechanical properties and low surface area of chitosan limit its application as an adsorbent. Various modifications, such as doping, amine modification, physical/chemical activation, impregnation, and composite formation, are used to enhance the CO2 capture performance of adsorbents [234]. The addition of various nanofillers, such as graphene-based materials and aerogel preparation, can be an effective solution. In this regard, Alhwaige et al. [241] prepared the chitosan aerogel composite with graphene oxide by using the freeze-drying method. They studied the effect of graphene oxide amount on the CO2 capture performance of composites. The increase in graphene oxide amounts results in increased surface area and CO2 capture performance. The prepared composite exhibits superior CO2 adsorption and high stability during prolonged cyclic operations.
Hsan et al. [242] prepared chitosan-grafted graphene oxide aerogels for CO2 adsorption. The CO2 capture of these aerogels reaches 0.257 mmol g−1, which is much higher than that of chitosan, at 1 bar. The developed low-cost aerogel can decrease the anthropogenic CO2 gas at favorable temperature and pressure. Kumar et al. [243] developed chitosan/graphene oxide nanocomposite film for environmental-friendly CO2 adsorption and its catalytic conversion to valuable products for industrial application. Polyvinyl amine/chitosan/graphene oxide membrane is prepared using the surface coating method for CO2 capture [244]. Results show that adding grafted graphene oxide as a nanofiller can enhance CO2/N2 selectivity of the membrane.
3.13 Biopolymer/graphene-based composites as adsorbent materials
The importance of water purification is known. Among various solutions, developing tailored nanocomposite membranes attracts huge attention. Natural abundant biopolymers, such as chitosan and cellulose, are considered due to their cost and biodegradability and are a concern in the development of new membranes.
Chen et al. [81] studied graphene derivative/bio-based polymer composite preparation methods and tailored their various properties for specified applications. Their utilization in separation applications, such as dye/organic separation and ion adsorption and separation, is studied.
Spoială et al. reviewed [245] the effect of different nanomaterials on chitosan-based nanocomposite membranes’ water purification performance.
Various strategies can be utilized to expand the adsorption properties of graphene-based materials on the basis of their composition, surface area, surface electrical structure, and spatial effect toward specific pollutants. The interaction mechanisms between pollutants and adsorbents are critical parameters to consider for improved adsorption performance. Wang et al. [246] studied the material design, performance, regeneration, and reuse of graphene-based functional material adsorbents; their associated adsorption mechanisms with heavy metal ions, dyes, and oils; and co-adsorption of their mixture from water. Various interactions, such as hydrophobic, van der Waals, electrostatic, complexation, π-interaction, and hydrogen bonding interactions, take place in the adsorption process. Considering that the material composition, morphology, structure, and functional groups on the adsorbent play a critical role in removal performance, Kong et al. [247] reviewed available methods for optimizing the heavy metal ions and their compound pollutant adsorption performance of graphene-based materials. Various modification methods to functionalize graphene-based adsorbents with various functional groups are studied for adsorbent optimization [247].
Biomass materials present interesting performance as biosorbents in wastewater remediation. Researchers utilized various modification techniques to improve their adsorption performance for dyes and heavy metals. H-bonding, chelation, electrostatic interaction, and π–π interactions are used for pollutant adsorption [248] Ahmed et al. [249] investigated different chitosan/chitin–carbonaceous material composites for the adsorption of various water pollutants and their regeneration and reusability as adsorbents.
Bacterial cellulose/graphene-based nanocomposites can be utilized as an adsorbent for water–oil separation and metal ion removal in water purification [11]. Their adsorption performance depends on various physicochemical properties, such as density, surface tension, viscosity, polarity, hydrophobicity, porosity, and pore size [250].
The development of super amphiphilic polyurethane/cellulose nanowhisker/graphene nanoplatelet foams with good reusability and durability leads to potential materials with an opportunity to be used in oil emulsion-purifying and catalyst-anchoring applications [251]. The development of a 3D magnetic bacterial cellulose nanofiber/graphene oxide polymer aerogel leads to an excellent adsorbent for malachite green with 93% removal performance [252]. Table 5 presents some recent studies conducted on the adsorbent application of biopolymer/graphene-based composites.
Some recent studies on depollution application
| Composite | Adsorbent | Preparation method | Ref. |
|---|---|---|---|
| Chitosan/graphene oxide composite aerogel | Methyl orange | Hydrothermal method | [253] |
| Cellulose nanofibril/graphene nanoplates hybrid aerogels | Cationic and anionic organic dyes | Freeze-drying | [254] |
| Chitosan/graphene oxide nanofibrous | Cu2+, Pb2+, and Cr6+ | Electrospinning | [255] |
| Metal ions | |||
| Immobilized horseradish peroxidase chitosan/graphene oxide nanocomposite | Ofloxacin | [256] | |
| Fe2O3–graphene oxide/chitosan composite | Cr6+ | Immersion–evaporation, coprecipitation | [257] |
| Schiff base chitosan/graphene oxide | Cu2+ and Pb2+ | [258] | |
| Chitosan/graphene oxide nanocomposite | Pb2+ | [259] | |
| Chitosan/aminopropylsilane graphene oxide nanocomposite hydrogel | Pb2+ and dyes | NIPS process | [260] |
| Chitosan-functionalized EDTA–silane/magnetic graphene oxide | Cd2+ and Pb2+ | Solvothermal | [261] |
4 Perspectives, challenges, and recommendations
The industry is waiting to absorb and implement the latest innovations and start manufacturing batteries, solar panels, electronics, photonic and communication devices, and medical technologies utilizing eco-friendly and sustainable materials. Biomedical applications are considered as the first mass applications to pave the way to emerging high value-added materials. Then, graphene can be incorporated in ubiquitous commodities, such as adsorbents, batteries, and electronics. However, the growth of biopolymer/graphene-based composite’s market is restrained by the price of production, competitive technologies, market fragmentation, and technical limitations.
Even with the development of various biopolymer/graphene oxides for medical applications, high purity is required to avoid toxicity and contamination and should be considered carefully. Thus, one of the important challenges for medical application is increasing the purity of prepared composites to avoid the side effects of other intermediates. Increased studies on developing bacteria-based nanocellulose can be a solution.
Modification plays a critical role in developing and increasing the performance of tailored biopolymer/graphene-based composites. Various physical and chemical modification methodologies can spearhead efforts to make initiatives in their fabrication to ensure consistency and trustworthiness.
The main goal of all studies is to see biopolymer/graphene-based composites fully integrated in day-to-day products and manufacturing. Based on the achievements and opportunities, future research trends can focus on the following:
Various modifications for graphene-based materials, biopolymers, and their composites for tailoring their structure, composition, and properties by considering interfacial interactions and processes and modification strategies that add value throughout the value chain (from new materials to individual components and products) to fulfill future industrial needs should be studied.
Finding a facile, rapid, green, and inexpensive way for large-scale preparation methods is important for commercialization and sustainability. Although several production routes for laboratory-scale have been reported, developing new ways to leverage versatility and unique properties of biopolymer/graphene-based composites should lead to continuous market growth.
The size control, uniformity, and compatibility based on the properties and performance of biopolymer/graphene-based composites are important and should be investigated.
Some properties and performance limitations of biopolymer/graphene-based composites can address by adding another building block or metal or metal oxide functionalization. Metal or metal oxide nanoparticles possess unique features and can alter chemical, electrical, magnetic, and conducting characteristics of targeted composite desirably.
The life cycle assessment is an important research area for innovative biopolymer/graphene-based composite materials for their industrialization. Studies should focus on potential differences in energy use, blue water footprint, human toxicity, and ecotoxicity of production routes. The life cycle assessment studies of products at early stages of technological development should be conducted in the future.
New composites, such as bioelastomer/graphene-based materials, with superior mechanical, electrical, and/or thermal behaviors for use as a biocompatible elastomer that provides structures with critical strengths for self-healing and 3D-printed scaffold should be developed.
Studies on minimally investigated areas, such as the effect of incorporation of biopolymer/graphene-based composites on cement, anticorrosion, and insulator coating materials, must be conducted.
5 Conclusion
Despite the different advantages of utilizing biopolymer/graphene-based composites in wide applications, such as medical, energy, adsorbent, electronic, and construction, their application is mostly limited to the laboratory scale. Research on understanding their various modification, size, and uniformity control and life cycle assessment should be carried out to overcome this issue and find easy, fast, green, and cheap methods for large-scale preparation. In the future, the increasing interest in developing engineered biopolymer/graphene-based composites with high performance and sustainability is expected to enhance their industrial application. Utilizing biomass wastes as precursors for developing biopolymer/graphene-based composites can enhance their cost effectiveness and eco-friendliness. We hope that this study provides some insight and inspiration for researchers in this field to develop green and sustainable biopolymer/graphene-based composites for various applications.
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Funding information: This study was partially supported by the FRGS/1/2019/TK10/UKM/02/1 and Universiti Kebangsaan Malaysia’s grant GP-K019259.
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Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.
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Conflicts of interest: The authors state no conflict of interest.
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- Thermal valuation and entropy inspection of second-grade nanoscale fluid flow over a stretching surface by applying Koo–Kleinstreuer–Li relation
- Mechanical properties and microstructure of nano-SiO2 and basalt-fiber-reinforced recycled aggregate concrete
- Characterization and tribology performance of polyaniline-coated nanodiamond lubricant additives
- Combined impact of Marangoni convection and thermophoretic particle deposition on chemically reactive transport of nanofluid flow over a stretching surface
- Spark plasma extrusion of binder free hydroxyapatite powder
- An investigation on thermo-mechanical performance of graphene-oxide-reinforced shape memory polymer
- Effect of nanoadditives on the novel leather fiber/recycled poly(ethylene-vinyl-acetate) polymer composites for multifunctional applications: Fabrication, characterizations, and multiobjective optimization using central composite design
- Design selection for a hemispherical dimple core sandwich panel using hybrid multi-criteria decision-making methods
- Improving tensile strength and impact toughness of plasticized poly(lactic acid) biocomposites by incorporating nanofibrillated cellulose
- Green synthesis of spinel copper ferrite (CuFe2O4) nanoparticles and their toxicity
- The effect of TaC and NbC hybrid and mono-nanoparticles on AA2024 nanocomposites: Microstructure, strengthening, and artificial aging
- Excited-state geometry relaxation of pyrene-modified cellulose nanocrystals under UV-light excitation for detecting Fe3+
- Effect of CNTs and MEA on the creep of face-slab concrete at an early age
- Effect of deformation conditions on compression phase transformation of AZ31
- Application of MXene as a new generation of highly conductive coating materials for electromembrane-surrounded solid-phase microextraction
- A comparative study of the elasto-plastic properties for ceramic nanocomposites filled by graphene or graphene oxide nanoplates
- Encapsulation strategies for improving the biological behavior of CdS@ZIF-8 nanocomposites
- Biosynthesis of ZnO NPs from pumpkin seeds’ extract and elucidation of its anticancer potential against breast cancer
- Preliminary trials of the gold nanoparticles conjugated chrysin: An assessment of anti-oxidant, anti-microbial, and in vitro cytotoxic activities of a nanoformulated flavonoid
- Effect of micron-scale pores increased by nano-SiO2 sol modification on the strength of cement mortar
- Fractional simulations for thermal flow of hybrid nanofluid with aluminum oxide and titanium oxide nanoparticles with water and blood base fluids
- The effect of graphene nano-powder on the viscosity of water: An experimental study and artificial neural network modeling
- Development of a novel heat- and shear-resistant nano-silica gelling agent
- Characterization, biocompatibility and in vivo of nominal MnO2-containing wollastonite glass-ceramic
- Entropy production simulation of second-grade magnetic nanomaterials flowing across an expanding surface with viscidness dissipative flux
- Enhancement in structural, morphological, and optical properties of copper oxide for optoelectronic device applications
- Aptamer-functionalized chitosan-coated gold nanoparticle complex as a suitable targeted drug carrier for improved breast cancer treatment
- Performance and overall evaluation of nano-alumina-modified asphalt mixture
- Analysis of pure nanofluid (GO/engine oil) and hybrid nanofluid (GO–Fe3O4/engine oil): Novel thermal and magnetic features
- Synthesis of Ag@AgCl modified anatase/rutile/brookite mixed phase TiO2 and their photocatalytic property
- Mechanisms and influential variables on the abrasion resistance hydraulic concrete
- Synergistic reinforcement mechanism of basalt fiber/cellulose nanocrystals/polypropylene composites
- Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
- Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
- Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
- Effects of nano-ZrSi2 on thermal stability of phenolic resin and thermal reusability of quartz–phenolic composites
- Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
- Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
- Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
- Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
- Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
- Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
- Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
- Mechanisms of the improved stiffness of flexible polymers under impact loading
- Anticancer potential of gold nanoparticles (AuNPs) using a battery of in vitro tests
- Review Articles
- Proposed approaches for coronaviruses elimination from wastewater: Membrane techniques and nanotechnology solutions
- Application of Pickering emulsion in oil drilling and production
- The contribution of microfluidics to the fight against tuberculosis
- Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
- Synthesis and encapsulation of iron oxide nanorods for application in magnetic hyperthermia and photothermal therapy
- Contemporary nano-architectured drugs and leads for ανβ3 integrin-based chemotherapy: Rationale and retrospect
- State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
- Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
- A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
- Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
- Advances in ZnO: Manipulation of defects for enhancing their technological potentials
- Efficacious nanomedicine track toward combating COVID-19
- A review of the design, processes, and properties of Mg-based composites
- Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
- Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
- Recent progress and challenges in plasmonic nanomaterials
- Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
- Electronic noses based on metal oxide nanowires: A review
- Framework materials for supercapacitors
- An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
- Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
- Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
- A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
- Recent advances in the preparation of PVDF-based piezoelectric materials
- Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
- Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
- Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
- Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
- Nanotechnology application on bamboo materials: A review
- Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
- Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
- 3D printing customized design of human bone tissue implant and its application
- Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
- A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
- Nanotechnology interventions as a putative tool for the treatment of dental afflictions
- Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
- A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
- Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
- Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
- Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
- Molecular dynamics application of cocrystal energetic materials: A review
- Synthesis and application of nanometer hydroxyapatite in biomedicine
- Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
- Biological applications of ternary quantum dots: A review
- Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
- Application of antibacterial nanoparticles in orthodontic materials
- Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
- Nanozymes – A route to overcome microbial resistance: A viewpoint
- Recent developments and applications of smart nanoparticles in biomedicine
- Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
- Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
- Diamond-like carbon films for tribological modification of rubber
- Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
- Recent research progress and advanced applications of silica/polymer nanocomposites
- Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
- Recent advances in perovskites-based optoelectronics
- Biogenic synthesis of palladium nanoparticles: New production methods and applications
- A comprehensive review of nanofluids with fractional derivatives: Modeling and application
- Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
- Electrohydrodynamic printing for demanding devices: A review of processing and applications
- Rapid Communications
- Structural material with designed thermal twist for a simple actuation
- Recent advances in photothermal materials for solar-driven crude oil adsorption
Articles in the same Issue
- Research Articles
- Theoretical and experimental investigation of MWCNT dispersion effect on the elastic modulus of flexible PDMS/MWCNT nanocomposites
- Mechanical, morphological, and fracture-deformation behavior of MWCNTs-reinforced (Al–Cu–Mg–T351) alloy cast nanocomposites fabricated by optimized mechanical milling and powder metallurgy techniques
- Flammability and physical stability of sugar palm crystalline nanocellulose reinforced thermoplastic sugar palm starch/poly(lactic acid) blend bionanocomposites
- Glutathione-loaded non-ionic surfactant niosomes: A new approach to improve oral bioavailability and hepatoprotective efficacy of glutathione
- Relationship between mechano-bactericidal activity and nanoblades density on chemically strengthened glass
- In situ regulation of microstructure and microwave-absorbing properties of FeSiAl through HNO3 oxidation
- Research on a mechanical model of magnetorheological fluid different diameter particles
- Nanomechanical and dynamic mechanical properties of rubber–wood–plastic composites
- Investigative properties of CeO2 doped with niobium: A combined characterization and DFT studies
- Miniaturized peptidomimetics and nano-vesiculation in endothelin types through probable nano-disk formation and structure property relationships of endothelins’ fragments
- N/S co-doped CoSe/C nanocubes as anode materials for Li-ion batteries
- Synergistic effects of halloysite nanotubes with metal and phosphorus additives on the optimal design of eco-friendly sandwich panels with maximum flame resistance and minimum weight
- Octreotide-conjugated silver nanoparticles for active targeting of somatostatin receptors and their application in a nebulized rat model
- Controllable morphology of Bi2S3 nanostructures formed via hydrothermal vulcanization of Bi2O3 thin-film layer and their photoelectrocatalytic performances
- Development of (−)-epigallocatechin-3-gallate-loaded folate receptor-targeted nanoparticles for prostate cancer treatment
- Enhancement of the mechanical properties of HDPE mineral nanocomposites by filler particles modulation of the matrix plastic/elastic behavior
- Effect of plasticizers on the properties of sugar palm nanocellulose/cinnamon essential oil reinforced starch bionanocomposite films
- Optimization of nano coating to reduce the thermal deformation of ball screws
- Preparation of efficient piezoelectric PVDF–HFP/Ni composite films by high electric field poling
- MHD dissipative Casson nanofluid liquid film flow due to an unsteady stretching sheet with radiation influence and slip velocity phenomenon
- Effects of nano-SiO2 modification on rubberised mortar and concrete with recycled coarse aggregates
- Mechanical and microscopic properties of fiber-reinforced coal gangue-based geopolymer concrete
- Effect of morphology and size on the thermodynamic stability of cerium oxide nanoparticles: Experiment and molecular dynamics calculation
- Mechanical performance of a CFRP composite reinforced via gelatin-CNTs: A study on fiber interfacial enhancement and matrix enhancement
- A practical review over surface modification, nanopatterns, emerging materials, drug delivery systems, and their biophysiochemical properties for dental implants: Recent progresses and advances
- HTR: An ultra-high speed algorithm for cage recognition of clathrate hydrates
- Effects of microalloying elements added by in situ synthesis on the microstructure of WCu composites
- A highly sensitive nanobiosensor based on aptamer-conjugated graphene-decorated rhodium nanoparticles for detection of HER2-positive circulating tumor cells
- Progressive collapse performance of shear strengthened RC frames by nano CFRP
- Core–shell heterostructured composites of carbon nanotubes and imine-linked hyperbranched polymers as metal-free Li-ion anodes
- A Galerkin strategy for tri-hybridized mixture in ethylene glycol comprising variable diffusion and thermal conductivity using non-Fourier’s theory
- Simple models for tensile modulus of shape memory polymer nanocomposites at ambient temperature
- Preparation and morphological studies of tin sulfide nanoparticles and use as efficient photocatalysts for the degradation of rhodamine B and phenol
- Polyethyleneimine-impregnated activated carbon nanofiber composited graphene-derived rice husk char for efficient post-combustion CO2 capture
- Electrospun nanofibers of Co3O4 nanocrystals encapsulated in cyclized-polyacrylonitrile for lithium storage
- Pitting corrosion induced on high-strength high carbon steel wire in high alkaline deaerated chloride electrolyte
- Formulation of polymeric nanoparticles loaded sorafenib; evaluation of cytotoxicity, molecular evaluation, and gene expression studies in lung and breast cancer cell lines
- Engineered nanocomposites in asphalt binders
- Influence of loading voltage, domain ratio, and additional load on the actuation of dielectric elastomer
- Thermally induced hex-graphene transitions in 2D carbon crystals
- The surface modification effect on the interfacial properties of glass fiber-reinforced epoxy: A molecular dynamics study
- Molecular dynamics study of deformation mechanism of interfacial microzone of Cu/Al2Cu/Al composites under tension
- Nanocolloid simulators of luminescent solar concentrator photovoltaic windows
- Compressive strength and anti-chloride ion penetration assessment of geopolymer mortar merging PVA fiber and nano-SiO2 using RBF–BP composite neural network
- Effect of 3-mercapto-1-propane sulfonate sulfonic acid and polyvinylpyrrolidone on the growth of cobalt pillar by electrodeposition
- Dynamics of convective slippery constraints on hybrid radiative Sutterby nanofluid flow by Galerkin finite element simulation
- Preparation of vanadium by the magnesiothermic self-propagating reduction and process control
- Microstructure-dependent photoelectrocatalytic activity of heterogeneous ZnO–ZnS nanosheets
- Cytotoxic and pro-inflammatory effects of molybdenum and tungsten disulphide on human bronchial cells
- Improving recycled aggregate concrete by compression casting and nano-silica
- Chemically reactive Maxwell nanoliquid flow by a stretching surface in the frames of Newtonian heating, nonlinear convection and radiative flux: Nanopolymer flow processing simulation
- Nonlinear dynamic and crack behaviors of carbon nanotubes-reinforced composites with various geometries
- Biosynthesis of copper oxide nanoparticles and its therapeutic efficacy against colon cancer
- Synthesis and characterization of smart stimuli-responsive herbal drug-encapsulated nanoniosome particles for efficient treatment of breast cancer
- Homotopic simulation for heat transport phenomenon of the Burgers nanofluids flow over a stretching cylinder with thermal convective and zero mass flux conditions
- Incorporation of copper and strontium ions in TiO2 nanotubes via dopamine to enhance hemocompatibility and cytocompatibility
- Mechanical, thermal, and barrier properties of starch films incorporated with chitosan nanoparticles
- Mechanical properties and microstructure of nano-strengthened recycled aggregate concrete
- Glucose-responsive nanogels efficiently maintain the stability and activity of therapeutic enzymes
- Tunning matrix rheology and mechanical performance of ultra-high performance concrete using cellulose nanofibers
- Flexible MXene/copper/cellulose nanofiber heat spreader films with enhanced thermal conductivity
- Promoted charge separation and specific surface area via interlacing of N-doped titanium dioxide nanotubes on carbon nitride nanosheets for photocatalytic degradation of Rhodamine B
- Elucidating the role of silicon dioxide and titanium dioxide nanoparticles in mitigating the disease of the eggplant caused by Phomopsis vexans, Ralstonia solanacearum, and root-knot nematode Meloidogyne incognita
- An implication of magnetic dipole in Carreau Yasuda liquid influenced by engine oil using ternary hybrid nanomaterial
- Robust synthesis of a composite phase of copper vanadium oxide with enhanced performance for durable aqueous Zn-ion batteries
- Tunning self-assembled phases of bovine serum albumin via hydrothermal process to synthesize novel functional hydrogel for skin protection against UVB
- A comparative experimental study on damping properties of epoxy nanocomposite beams reinforced with carbon nanotubes and graphene nanoplatelets
- Lightweight and hydrophobic Ni/GO/PVA composite aerogels for ultrahigh performance electromagnetic interference shielding
- Research on the auxetic behavior and mechanical properties of periodically rotating graphene nanostructures
- Repairing performances of novel cement mortar modified with graphene oxide and polyacrylate polymer
- Closed-loop recycling and fabrication of hydrophilic CNT films with high performance
- Design of thin-film configuration of SnO2–Ag2O composites for NO2 gas-sensing applications
- Study on stress distribution of SiC/Al composites based on microstructure models with microns and nanoparticles
- PVDF green nanofibers as potential carriers for improving self-healing and mechanical properties of carbon fiber/epoxy prepregs
- Osteogenesis capability of three-dimensionally printed poly(lactic acid)-halloysite nanotube scaffolds containing strontium ranelate
- Silver nanoparticles induce mitochondria-dependent apoptosis and late non-canonical autophagy in HT-29 colon cancer cells
- Preparation and bonding mechanisms of polymer/metal hybrid composite by nano molding technology
- Damage self-sensing and strain monitoring of glass-reinforced epoxy composite impregnated with graphene nanoplatelet and multiwalled carbon nanotubes
- Thermal analysis characterisation of solar-powered ship using Oldroyd hybrid nanofluids in parabolic trough solar collector: An optimal thermal application
- Pyrene-functionalized halloysite nanotubes for simultaneously detecting and separating Hg(ii) in aqueous media: A comprehensive comparison on interparticle and intraparticle excimers
- Fabrication of self-assembly CNT flexible film and its piezoresistive sensing behaviors
- Thermal valuation and entropy inspection of second-grade nanoscale fluid flow over a stretching surface by applying Koo–Kleinstreuer–Li relation
- Mechanical properties and microstructure of nano-SiO2 and basalt-fiber-reinforced recycled aggregate concrete
- Characterization and tribology performance of polyaniline-coated nanodiamond lubricant additives
- Combined impact of Marangoni convection and thermophoretic particle deposition on chemically reactive transport of nanofluid flow over a stretching surface
- Spark plasma extrusion of binder free hydroxyapatite powder
- An investigation on thermo-mechanical performance of graphene-oxide-reinforced shape memory polymer
- Effect of nanoadditives on the novel leather fiber/recycled poly(ethylene-vinyl-acetate) polymer composites for multifunctional applications: Fabrication, characterizations, and multiobjective optimization using central composite design
- Design selection for a hemispherical dimple core sandwich panel using hybrid multi-criteria decision-making methods
- Improving tensile strength and impact toughness of plasticized poly(lactic acid) biocomposites by incorporating nanofibrillated cellulose
- Green synthesis of spinel copper ferrite (CuFe2O4) nanoparticles and their toxicity
- The effect of TaC and NbC hybrid and mono-nanoparticles on AA2024 nanocomposites: Microstructure, strengthening, and artificial aging
- Excited-state geometry relaxation of pyrene-modified cellulose nanocrystals under UV-light excitation for detecting Fe3+
- Effect of CNTs and MEA on the creep of face-slab concrete at an early age
- Effect of deformation conditions on compression phase transformation of AZ31
- Application of MXene as a new generation of highly conductive coating materials for electromembrane-surrounded solid-phase microextraction
- A comparative study of the elasto-plastic properties for ceramic nanocomposites filled by graphene or graphene oxide nanoplates
- Encapsulation strategies for improving the biological behavior of CdS@ZIF-8 nanocomposites
- Biosynthesis of ZnO NPs from pumpkin seeds’ extract and elucidation of its anticancer potential against breast cancer
- Preliminary trials of the gold nanoparticles conjugated chrysin: An assessment of anti-oxidant, anti-microbial, and in vitro cytotoxic activities of a nanoformulated flavonoid
- Effect of micron-scale pores increased by nano-SiO2 sol modification on the strength of cement mortar
- Fractional simulations for thermal flow of hybrid nanofluid with aluminum oxide and titanium oxide nanoparticles with water and blood base fluids
- The effect of graphene nano-powder on the viscosity of water: An experimental study and artificial neural network modeling
- Development of a novel heat- and shear-resistant nano-silica gelling agent
- Characterization, biocompatibility and in vivo of nominal MnO2-containing wollastonite glass-ceramic
- Entropy production simulation of second-grade magnetic nanomaterials flowing across an expanding surface with viscidness dissipative flux
- Enhancement in structural, morphological, and optical properties of copper oxide for optoelectronic device applications
- Aptamer-functionalized chitosan-coated gold nanoparticle complex as a suitable targeted drug carrier for improved breast cancer treatment
- Performance and overall evaluation of nano-alumina-modified asphalt mixture
- Analysis of pure nanofluid (GO/engine oil) and hybrid nanofluid (GO–Fe3O4/engine oil): Novel thermal and magnetic features
- Synthesis of Ag@AgCl modified anatase/rutile/brookite mixed phase TiO2 and their photocatalytic property
- Mechanisms and influential variables on the abrasion resistance hydraulic concrete
- Synergistic reinforcement mechanism of basalt fiber/cellulose nanocrystals/polypropylene composites
- Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
- Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
- Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
- Effects of nano-ZrSi2 on thermal stability of phenolic resin and thermal reusability of quartz–phenolic composites
- Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
- Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
- Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
- Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
- Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
- Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
- Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
- Mechanisms of the improved stiffness of flexible polymers under impact loading
- Anticancer potential of gold nanoparticles (AuNPs) using a battery of in vitro tests
- Review Articles
- Proposed approaches for coronaviruses elimination from wastewater: Membrane techniques and nanotechnology solutions
- Application of Pickering emulsion in oil drilling and production
- The contribution of microfluidics to the fight against tuberculosis
- Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
- Synthesis and encapsulation of iron oxide nanorods for application in magnetic hyperthermia and photothermal therapy
- Contemporary nano-architectured drugs and leads for ανβ3 integrin-based chemotherapy: Rationale and retrospect
- State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
- Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
- A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
- Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
- Advances in ZnO: Manipulation of defects for enhancing their technological potentials
- Efficacious nanomedicine track toward combating COVID-19
- A review of the design, processes, and properties of Mg-based composites
- Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
- Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
- Recent progress and challenges in plasmonic nanomaterials
- Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
- Electronic noses based on metal oxide nanowires: A review
- Framework materials for supercapacitors
- An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
- Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
- Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
- A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
- Recent advances in the preparation of PVDF-based piezoelectric materials
- Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
- Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
- Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
- Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
- Nanotechnology application on bamboo materials: A review
- Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
- Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
- 3D printing customized design of human bone tissue implant and its application
- Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
- A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
- Nanotechnology interventions as a putative tool for the treatment of dental afflictions
- Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
- A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
- Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
- Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
- Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
- Molecular dynamics application of cocrystal energetic materials: A review
- Synthesis and application of nanometer hydroxyapatite in biomedicine
- Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
- Biological applications of ternary quantum dots: A review
- Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
- Application of antibacterial nanoparticles in orthodontic materials
- Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
- Nanozymes – A route to overcome microbial resistance: A viewpoint
- Recent developments and applications of smart nanoparticles in biomedicine
- Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
- Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
- Diamond-like carbon films for tribological modification of rubber
- Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
- Recent research progress and advanced applications of silica/polymer nanocomposites
- Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
- Recent advances in perovskites-based optoelectronics
- Biogenic synthesis of palladium nanoparticles: New production methods and applications
- A comprehensive review of nanofluids with fractional derivatives: Modeling and application
- Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
- Electrohydrodynamic printing for demanding devices: A review of processing and applications
- Rapid Communications
- Structural material with designed thermal twist for a simple actuation
- Recent advances in photothermal materials for solar-driven crude oil adsorption
