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Microstructure-dependent photoelectrocatalytic activity of heterogeneous ZnO–ZnS nanosheets

  • Yuan-Chang Liang EMAIL logo and Chia-Hung Huang
Published/Copyright: March 14, 2022
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Nanotechnology Reviews
From the journal Nanotechnology Reviews Volume 11 Issue 1

Abstract

ZnS crystallite-loaded ZnO sheet composites were successfully synthesized through vulcanization of hydrothermally derived porous ZnO sheet templates. The sulfur precursor (Na2S: 0.05–0.25 M) concentration affects the ZnS loading content and surface morphology of the ZnO–ZnS composites. A higher sulfur precursor concentration increased the ZnS loading content and decreased the porosity of the ZnO–ZnS composites. The ZnO–ZnS sheet composites with the atomic composition ratio of ZnO larger than that of the decorated ZnS exhibited an enhanced photoactivity. By contrast, the overloading of ZnS crystallites on the ZnO template decreased photoactivity. The ZnO–ZnS sheet composite with a S/O atomic ratio of 0.61 exhibits the highest photoactivity among various samples. The enhanced charge separation efficiency because of the formation of ZnO/ZnS heterojunctions and porous structure allowed the synthesis of the ZnO–ZnS composite via hydrothermal vulcanization with 0.05 M Na2S, and shows the higher photoelectrochemical (PEC) degradation ability towards Rhodamine B solution among various samples. The scavenger tests and the proposed PEC-degradation mechanism demonstrate that superoxide radicals are the main active species for the degradation of the RhB solution. The experimental results herein show that the porous ZnO–ZnS sheet composite with a suitable phase ratio is promising for photoelectrocatalyst applications.

Keywords: sheet composite; microstructure; photoactive performance

1 Introduction

ZnO is widely used for degrading organic pollutants due to its variety of preparation methods, low cost, nontoxicity, and strong redox ability [1,2]. Several routes have been established for the synthesis of low-dimensional ZnO crystals with various morphologies, such as hydrothermal method, chemical bath deposition, vapor deposition, and sputtering deposition [3,4,5,6]. It has been shown that the advantages of a high specific surface area, abundant surface active sites, and strong adsorption capacity make low-dimensional ZnO nanomaterials suitable for catalytic reaction applications. Recently, the development of porous ZnO nanostructures shows that the tiny pores in ZnO substantially improve their specific surface area size, light absorption ability, and surface active site number in comparison with the ZnO with solid crystal characteristics [3,7]. Therefore, porous ZnO nanomaterials are a good candidate for use in photoactive devices with high performance. Furthermore, ZnS because of its remarkable chemical stability against oxidation and hydrolysis also receives much attention for application in photoactive devices [8]. Great efforts have been steadily devoted to synthesize ZnS nanostructures, aiming to enhance their photoactive performance via controlling their specific surface area and photoinduced charge separation efficiency. Several approaches have been adopted for synthesizing ZnS nanostructures with different morphologies for high-performance applications in photoactive devices [9,10].

Photocatalytic activation of semiconductors is mainly dominated by the number of excitons under irradiation to generate free radicals to degrade target pollutants [11,12,13,14,15,16,17]. Therefore, the control of photoinduced charge separation efficiency is a key for ZnO or ZnS to perform high photocatalytic performance. Several approaches including the incorporation of impurity, crystal defect, and formation of a heterostructure have been widely adopted for ZnO or ZnS for improved photoactive performance [18,19,20]. Among these approaches, the formation of ZnO- or ZnS-based heterostructures with a suitable band alignment between the constituent compounds is of potential importance to enhance the photoactive performance of ZnO or ZnS. This is due to various choices of coupling semiconductors to be integrated into the ZnO or ZnS, and the formation of a heterostructure has a high degree of freedom to manipulate the photoactive performance of the semiconductors. More importantly, due to the suitable Type II band alignment between the ZnO and ZnS, the construction of the ZnO/ZnS heterostructure has been shown to be a promising combination to improve the photoactive performance of the constituent counterparts [21].

The morphology, microstructure, composition ratio, and band alignment are factors that affect the final photoactive performance of the ZnO–ZnS heterostructures [22,23]. The control of ZnO–ZnS heterostructures with abundant active surfaces and interfaces for the photocatalytic process and design of the heterojunction to promote the separation and transfer of photogenerated electrons and holes with suitable bandgap positions are still a challenge to synthesize ZnO–ZnS composites with high photoactive performance. In this study, porous ZnO–ZnS sheet-like nanostructures are synthesized using a hydrothermal vulcanization method with porous ZnO sheet templates. The porous ZnO sheet templates can improve photocatalytic activity due to their high specific surface area. Moreover, the formation of ZnO–ZnS porous nanosheets by varying the parameters of hydrothermal vulcanization utilizes the control of microstructures of the ZnO–ZnS sheet composites to obtain high photoactive performance at a low-temperature and low-cost process. The systematic investigation on the vulcanization process-dependent microstructure evolution of ZnO–ZnS sheet composites in this study provides a promising approach to synthesize and design ZnO–ZnS sheet composites for photoelectrocatalytic device applications with high efficiency.

2 Experiments

2.1 Preparation of porous ZnO nanosheet templates

The ZnO nanosheets were grown on an F-doped tin oxide (FTO) glass substrate by the hydrothermal approach. A 100 mL aqueous solution consisting of zinc nitrate hexahydrate (Zn(NO3)2·6H2O; 4.477 g) and urea ((NH2)2CO; 16.67 g) dissolved in it was used as a precursor solution. The hydrothermal reaction was performed at 90°C for 4 h in this study. After the hydrothermal deposition, template products identified as Zn4CO3(OH)6·H2O nanosheets were formed. The template nanosheet products were further annealed at 400℃ for 30 min in ambient air to form a crystalline porous ZnO nanosheet template.

2.2 Preparation of ZnO–ZnS heterostructures

ZnO–ZnS heterostructures were prepared by the hydrothermal vulcanization method. The ZnO nanosheet templates were immersed in 0.05, 0.1, and 0.25 M Na2S·9H2O dissolved solutions, respectively. The samples for the ZnO template treated with 0.05, 0.1, and 0.25 M Na2S·9H2O are named ZS-1, ZS-2, and ZS-3, respectively. The hydrothermal reaction was performed at 70℃ for 2 h. For band energy evaluation, the pure ZnS nanosheets were further made using 0.5 M Na2S·9H2O solution for hydrothermal vulcanization of the ZnO nanosheet template. The final products were washed with deionized water and dried at 60℃ in a drying oven for 24 h.

2.3 Material analysis and characterization tests

The crystallographic structures of the products were characterized by X-ray diffraction (XRD) using a Bruker D2 PHASER. The morphologies of the products were investigated using field emission scanning electron microscopy (FE-SEM; JEOL JSM-7900F). High-resolution lattice images, composition, and selected area electron diffraction of the products were recorded using high-resolution transmission electron microscopy (HR-TEM; JEOL JEM-2100F) equipped with an energy-dispersive X-ray spectroscope (EDS). X-ray photoelectron spectroscopy (XPS; PHI 5000 VersaProbe) was used to analyze the elemental binding energies of the products. The analysis of absorbance spectra of the products was conducted using a UV-Vis spectrophotometer (Jasco V750).

The photoelectrochemical (PEC) and impedance spectroscopy properties of the products were characterized in a three-electrode electrochemical quartz cell using an electrochemical analyzer (SP-150, BioLogic). The as-synthesized product was used as the working electrode as well as a Pt wire and an Ag/AgCl electrode were used as the counter electrode and reference electrode, respectively. The electrolyte is a 0.5 M Na2SO4 solution and the irradiation source for measurements is excited with a 100 W Xe arc lamp. The light intensity on the sample is approximately 3.12 mW/cm2. The photoelectrocatalytic activities of the products were evaluated by PEC-degrading rhodamine B (RhB) solution with different irradiation durations of 15, 30, 45, and 60 min. Moreover, the dark balance absorption tests of various samples for 30 min are also conducted. A total of 10 mL of RhB solution (10−5) M was added to 10 mL of 0.5 M Na2SO4 solution to form a homogeneous aqueous solution for PEC-degradation system use, and the applied potential was varied from 0 to 1 V during PEC-degradation tests. The concentration of the degraded RhB solution was evaluated by recording the absorbance spectra intensity variation ratio of the RhB solution before and after the test. The C t /C 0 is evaluated from I t /I 0, in which C 0 is the initial concentration of the RhB solution, C t is the concentration of that at a different interval during the degradation process, I 0 is the absorbance spectrum intensity of the initial RhB solution, and I t is the absorbance spectrum intensity of the RhB solution at a different interval during the degradation process.

3 Results and discussion

Figure 1(a) shows the porous ZnO nanosheet template. The sheet thickness is approximately 20 nm. Moreover, numerous tiny nanoscaled pores existed in the sheet. Figure 1(b) and (c) display the morphology of the porous ZnO nanosheet template treated with different vulcanization processes with various sulfur precursor concentrations of 0.05 M, 0.1 M, and 0.25 M Na2S. Figure 1(b) and (c) indicate that the morphology of the ZnO nanosheet template did not show a marked change after the vulcanization process with the lower sulfur concentration below 0.1 M. The sheet template still maintained a porous structure with abundant tiny pores on it. Notably, when the sulfur precursor concentration was substantially increased to 0.25 M, the morphology changed to be more solid, and no distinct porous structure was observed for the ZnO sheet template after vulcanization. The addition of Na2S into the hydrothermal reaction solution results in the ion exchange between S2− from the dissolved Na2S and O2− from the ZnO template, and this ion exchange process promotes the formation of ZnS crystallites on the surfaces of the ZnO sheet template [24,25,26]. The inward diffusion of S2− to interact with Zn2+ in the ZnO template forms the ZnS phase during the hydrothermal vulcanization process. Notably, even the vulcanization process was conducted for the ZnO sheet template with an increased sulfur precursor concentration ranging from 0.01 to 0.25 M, the sheet-like feature of the ZnO template was still maintained in this study, revealing a gradual dissolve of the ZnO phase and the formation of ZnS phase reached an equilibrium state during the current hydrothermal vulcanization processes. With the increase of the sulfur ion source, more ZnO might convert into ZnS with an increased reaction degree of ion exchange, and the generated ZnS crystallites will cover the residual ZnO surface and reorganize the surface topography of the porous ZnO sheet template. Therefore, the porous ZnO sheet template treated with the highest sulfur concentration herein causes more ZnS crystallites to form, leading to the disappearance of the porous surface of the ZnO sheet template.

Figure 1 SEM images of various products: (a) ZnO template, (b) ZS-1, (c) ZS-2, and (d) ZS-3.
Figure 1

SEM images of various products: (a) ZnO template, (b) ZS-1, (c) ZS-2, and (d) ZS-3.

Figure 2 shows the XRD patterns of the ZnO sheet template treated with and without various vulcanization processes. In Figure 2(a), in addition to FTO Bragg reflections, the distinct and intense Bragg reflections centered at 31.77°, 34.42°, 36.25°, 47.54°, and 56.6° are characteristics to wurtzite ZnO (100), (002), (101), (102), and (110) planes according to JCPDS No. 36-1451. The substantially intense nonpolar crystallographic planes of (100) and (101) and weak intensity of the c-axis crystal plane (002) reveal the sheet morphological feature of the ZnO herein [3,27]. When the ZnO sheet template was treated with the vulcanization process, additional new Bragg reflections centered at 28.56°, 47.51°, and 56.29° are observed and ascribed to the cubic ZnS (111), (220), and (311) crystal planes according to JCPDS No. 05-0566 in Figure 2(b)–(d). Notably, the ZnO( 102) and (110) positions are close to those of the ZnS (220) and (311), respectively. However, the markedly decreased intensity and broadened peak width of the Bragg reflections centered at approximately 47.51–47.54° and 56.29–56.6° might reveal the overlap of the Bragg reflections of the ZnO and ZnS phase planes in these two theta angle regions. The XRD results reveal that the vulcanization processes herein are effective to induce the partial ZnO template crystal to transfer into the ZnS phase. Furthermore, the intensity of the characteristic crystallographic plane of cubic ZnS (111) was substantially increased with the increased sulfur precursor concentration, revealing an increased content of ZnS crystals in the sample [21,26]. From the comparison and investigation of the main characteristic crystallographic planes (100) and (101) of the ZnO sheet and (111) of ZnS crystals, the ZS-1, ZS-2, and ZS-3 show the clear coexistence of ZnO and ZnS phases in the products and are in a crystalline composite structure. Notably, the substantially weak Bragg reflections of ZnO( 100) and (101) together with a markedly intense Bragg reflection of ZnS (111) in Figure 2(d) demonstrates that the ZnO template has been massively vulcanized for the ZS-3.

Figure 2 XRD patterns of various products: (a) ZnO template, (b) ZS-1, (c) ZS-2, and (d) ZS-3. The ZnO and ZnS crystallographic planes are marked with black and blue, respectively.
Figure 2

XRD patterns of various products: (a) ZnO template, (b) ZS-1, (c) ZS-2, and (d) ZS-3. The ZnO and ZnS crystallographic planes are marked with black and blue, respectively.

Figure 3(a) shows the low-magnification TEM image of the ZS-1 nanosheet. Visible pores in a nanometer scale existed in the sheet structure, and the diameter of the sheet is approximately 1 µm. The HRTEM images taken from the outer and inner pore regions of the sheet are displayed in Figure 3(b)–(e). The visible lattice fringes arranged with an interval of 0.31 nm corresponded well to the interplanar spacing of the (111) plane of the cubic ZnS structure. Moreover, some inner regions of the HR images displayed twisted and overlapped lattice fringes that might be associated with the overlapped crystals of ZnO and ZnS. Figure 3(f) demonstrates the selected-area electron diffraction (SAED) pattern of the ZS-1 nanosheet. The SAED pattern revealed a multiringed, multiphase pattern with ZnO (002), (102), (200) and ZnS (111), (311). The SAED pattern presents the coexistence of ZnO and ZnS in the ZS-1 nanosheet and the result is consistent with the aforementioned XRD pattern. The EDS spectra in Figure 3(g) clarify the elemental composition of the ZS-1 nanosheet. In addition to Cu and C signals from the TEM grid, no impurity elements are detected herein. The atomic percentages of Zn, O, and S for the ZS-1 nanosheet is 48, 32.2, and 19.8, respectively. Furthermore, the spatial elemental distribution of Zn, S, and O in the ZS-1 sheet structure is shown in Figure 3(h). The elemental distribution of Zn, O, and S atoms over the selected nanosheet reveals that the ZS-1 has a homogeneous composition of ZnO and ZnS that coexisted in the nanosheet.

Figure 3 TEM analysis of the ZS-1: (a) low-magnification image. (b)–(e) HRTEM images of various local regions in image (a). (f) SAED pattern. (g) EDS spectrum. (h) Elemental mapping images.
Figure 3

TEM analysis of the ZS-1: (a) low-magnification image. (b)–(e) HRTEM images of various local regions in image (a). (f) SAED pattern. (g) EDS spectrum. (h) Elemental mapping images.

Similarly, the ZS-2 nanosheet also presents a porous sheet structure in Figure 4(a). The existence of lattice fringes of ZnS (111) is also demonstrated in the outer regions of the selected HR images in Figure 4(b) and (c). Moreover, overlapped and twisted lattice fringes characterized by the coexistence of the ZnO and ZnS phases are presented in HR images. The EDS spectra in Figure 4(d) reveal that the atomic percentages of Zn, O, and S are approximately 57.5, 23.0, and 19.5, respectively for the ZS-2 nanosheet.

Figure 4 TEM analysis of the ZS-2: (a) low-magnification image. (b) and (c) HRTEM images of various local regions in image (a). (d) EDS spectrum.
Figure 4

TEM analysis of the ZS-2: (a) low-magnification image. (b) and (c) HRTEM images of various local regions in image (a). (d) EDS spectrum.

Figure 5(a) represents the low-magnification TEM image of the ZS-3 nanosheet. The ZS-3 nanosheet has a different surface feature from those of ZS-1 and ZS-2. The ZS-3 nanosheet has a dense and particle aggregated surface feature. No pores are visibly distinguished in the ZS-3. From Figure 5(b) and (c), the HRTEM micrograph indicated clear ZnS (111) lattice fringes. The grayscale comparison in these HR images presents clear particle aggregated features at the peripheral region of the nanosheet. This might be associated with an increased crystalline quality of ZnS crystallites at the given vulcanization process [26]. The SAED pattern in Figure 5(d) shows ZnO (002) and (103), ZnS (111), (220), and (103) planes, revealing that the ZS-3 consisted of ZnO and ZnS phases. From the EDS spectra of the ZS-3 (Figure 5(e)) the Zn, O, and S atomic percentages of the ZS-3 are found to be 62.0, 8.2, and 29.8%, respectively. Notably, the summarized compositions comparison of the S/O atomic ratio from TEM-EDS spectra for ZS-1, ZS-2, and ZS-3 are 0.61, 0.85, and 3.63, respectively, highlighting that more ZnO crystals were converted into the ZnS phase with an increased sulfur precursor concentration during the vulcanization process.

Figure 5 TEM analysis of the ZS-3: (a) low-magnification image. (b) and (c) HRTEM images of various local regions in image (a). (d) SAED pattern. (e) EDS spectrum.
Figure 5

TEM analysis of the ZS-3: (a) low-magnification image. (b) and (c) HRTEM images of various local regions in image (a). (d) SAED pattern. (e) EDS spectrum.

The narrow scan XPS spectra of Zn2p regions for the ZS-1, ZS-2, and ZS-3 are presented in Figure 6(a)–(c), respectively. The Zn2p3/2 and Zn2p1/2 peaks are centered at approximately 1021.1 and 1044.1 eV, respectively. The spin–orbit splitting of approximately 23 eV between the Zn2p3/2 and Zn2p1/2 core–level components reveals the Zn2+ state nature herein [21,28]. Notably, the core–level Zn2p binding energies of Zn–O are close to those of Zn–S [21]. Due to the similar Zn2+ binding energy of ZnO and ZnS phases, there are no substantial differences in the obtained Zn2p spectra among various samples. Figure 6(d)–(f) presents XPS S2p spectra of various samples. Notably, asymmetric S2p spectra can be further deconvoluted into two subpeaks that are centered at approximately 161.1 and 162.1 eV and are attributed to S2p3/2 and S2p1/2 of S2− binding states, respectively [21,25]. Moreover, the peak intensity ratio of S2p1/2 to S2p3/2 was approximately 1:2, revealing that the ZnS phase has been successfully synthesized by O2− and S2− ion exchange during the given vulcanization processes for the ZnO sheet template. Moreover, the higher S2p spectrum intensity of ZS-3 reveals higher content of the ZnS phase in the ZS-3 composite. The O1s XPS spectra of ZS-1, ZS-2, and ZS-3 are shown in Figure 6(g)–(i), respectively. The decreased O1s spectrum intensity for the composite structure with an increased sulfur precursor concentration demonstrates an increased sulfidation degree of the ZnO template to form more Zn–S bonds [29]. The O1s spectra are further split into two subpeaks. The subpeak centered at approximately 530.7 eV (blue line) is assigned to the crystal lattice oxygen ions in ZnO, and the peak centered at approximately 531.5 eV (green line) is associated with the oxygen vacancy and/or absorbed OH− in the ZnO lattice [30]. The XPS results herein reveal that a composite structure of ZnO–ZnS was formed for the ZS-1, ZS-2, and ZS-3 samples.

Figure 6 High-resolution XPS spectra in Zn2p: (a) ZS-1, (b) ZS-2, and (c) ZS-3. High-resolution XPS spectra in S2p: (d) ZS-1, (e) ZS-2, and (f) ZS-3. High-resolution XPS spectra in O1s: (g) ZS-1, (h) ZS-2, and (i) ZS-3.
Figure 6

High-resolution XPS spectra in Zn2p: (a) ZS-1, (b) ZS-2, and (c) ZS-3. High-resolution XPS spectra in S2p: (d) ZS-1, (e) ZS-2, and (f) ZS-3. High-resolution XPS spectra in O1s: (g) ZS-1, (h) ZS-2, and (i) ZS-3.

The optical absorption spectra of various samples are shown in Figure 7(a). It can be clearly seen that the ZnO template has a strong absorption edge at approximately 380 nm. The optical absorption edge gradually shifted to a shorter wavelength for the ZnO template treated by vulcanization processes with an increased sulfur precursor concentration. Notably, dual optical absorption edges are visibly observed for the ZS-1, ZS-2, and ZS-3. The dual absorption edges are associated with the contribution of two constituent phases of ZnO and ZnS, and this has also been demonstrated in the ZnO–ZnS heterostructure synthesized via a solid-state low-temperature synthesis method [31]. Moreover, from Figure 7(a), all the prepared products have optical absorption edges located in the UV range, revealing they are UV-light sensitizer materials. The band gap energy (E g) of the products can be further calculated according to the equation (αhv)2 = A(hv − E g), where A is a constant, E g is the band gap energy, h is the Planck constant, and α is the absorption coefficient. Figure 7(b) and (c) illustrate the (αhv)2 versus photon energy plots used for the evaluation of the band gap energy of the constituent semiconductors. The band gap energy was estimated to be approximately 3.2 eV for ZnO [27] and 3.4 eV for ZnS herein. The evaluated ZnS band gap energy is close to the reported value of ZnS nanoparticles synthesized via wet chemical methods [32]. Moreover, Figure 7(c) reveals the coexistence of the band gap energies of ZnO and ZnS phases; this is in agreement with the previous structural analysis of ZS-3 associated with the formation of the ZnO–ZnS composite structure.

Figure 7 (a) UV-Vis absorption spectra of various products. (b) The band gap evaluation of the ZnO template. (c) The band gap evaluation of ZS-3.
Figure 7

(a) UV-Vis absorption spectra of various products. (b) The band gap evaluation of the ZnO template. (c) The band gap evaluation of ZS-3.

The cycling photocurrent density versus time (I–t) curves under chopping irradiation for ZnO, ZS-1, ZS-2, and ZS-3 are shown in Figure 8(a). The average photocurrent densities of ZnO, ZS-1, ZS-2, and ZS-3 photoelectrodes are approximately 0.61, 1.22, 1.06, and 0.23 mA/cm2 at 0.5 V vs Ag/AgCl. The ZS-1 shows the highest photocurrent density at the test cycles. Moreover, both the ZS-1 and ZS-2 exhibit a higher photoresponse than that of the ZnO template, implying improved charge separation and transfer abilities in the ZS-1 and ZS-2. By contrast, the ZS-3 demonstrates the deteriorated photoresponse performance in comparison with that of the pristine ZnO. The result reveals that the content of ZnS in the ZnO–ZnS composite affects the photo-induced charge separation efficiency in the composite structure. The fewer ZnS crystallites in the porous ZnO–ZnS sheet-like composite structure improves the separation of electron–hole pairs between ZnO and ZnS under irradiation, and thus, have a better photoresponse. By contrast, the photo-induced electron–hole pairs are unable to be separated effectively for massive ZnS crystallites in the solid ZnO–ZnS sheet-like composite structure. It has been shown that the thick ZnS shell layer in the ZnO–ZnS core–shell nanofibers suppresses the tunneling efficiency of the holes from the ZnO core to the ZnS shell [29], and this work supports the observed deteriorated photoresponse performance of the ZS-3 herein. Notably, the photocorrosion phenomenon was observed from the ZS-1 and ZS-2 composites. The photocorrosion causes the slightly decreased photocurrent with the irradiation on/off cyclic number, and this phenomenon might be associated with the accumulation of excessive light-induced holes on the ZnS surface at the given test condition [33]. Figure 8(b) shows the Nyquist plots of various products. Comparatively, the ZS-1 displays the smallest semicircle radius among various products. The smaller radius of the Nyquist plot’s semicircle implies lower interfacial charge transfer resistance in semiconductor heterostructures [34,35,36]. The corresponding equivalent circuits for the pristine ZnO template and ZnO–ZnS composite are shown in Figure 8(c). Notably, R s represents the series resistance of the electrochemical device. C s and R CTs represent the capacitance phase element and charge transfer resistance of the depletion layer of the semiconductor, respectively. C d and R CT are the capacitance phase element and the charge transfer resistance at the double layer of the semiconductor–electrolyte interface, respectively [37]. According to the fitting results from the Nyquist plots using the proposed circuit models, the R CT is approximately 6,510, 2,594, 3,566, and 12,665 Ω for the pristine ZnO, ZS-1, ZS-2, and ZS-3 respectively. The smaller R CT of ZS-1 is ascribed to a faster charge transfer and higher separation rate of photogenerated electron–hole pairs in the composite structure [34], which supports the aforementioned photoresponse performance of the samples. Similarly, in ZnS or ZnIn2S4-modified ZnO nanorods, the decoration of suitable sulfides substantially decreases the R CT of the ZnO–sulfides system, and therefore, obtains an enhanced photoresponse in comparison with the pristine ZnO nanorods [38]

Figure 8 (a) Chronoamperometric I–t curves collected at 0.5 V vs Ag/AgCl for various products under chopping irradiation. (b) Nyquist plots of various products under irradiation. (c) The possible equivalent circuits employed to fit the Nyquist plots of various products. The upper one is for the ZnO template, and the lower one is for the ZnO–ZnS composites.
Figure 8

(a) Chronoamperometric I–t curves collected at 0.5 V vs Ag/AgCl for various products under chopping irradiation. (b) Nyquist plots of various products under irradiation. (c) The possible equivalent circuits employed to fit the Nyquist plots of various products. The upper one is for the ZnO template, and the lower one is for the ZnO–ZnS composites.

Figure 9(a) shows the Mott–Schottky (M–S) plots of the pristine ZnO template. The positive slope in the M–S plots indicates the n-type nature of ZnO [27]. Moreover, the flat band potential at the electrolyte/electrode interface can be estimated from the M–S curves according to the M–S equation [34]. By extrapolating the X-axis intercepts of the linear region in the M–S curve, the flat band potential of ZnO has been determined to be approximately −0.5 eV (vs NHE). The evaluated value is close to the hydrothermally derived ZnO nanorods that have a flat band potential of −0.55 V (vs NHE) [39]. Compared with the flat band potential of the ZnO template, the value of the representative ZnO–ZnS heterogeneous structure (ZS-1) was more negative in Figure 9(b). The flat band potential of ZS-1 is estimated to be −0.63 eV. A more negative flat band reflects a smaller barrier to the charge transfer and can induce more electrons accumulation in the conduction band of the sample, thus suppressing the recombination of photogenerated electron–hole pairs [40]. A negative shift of the flat band level of the ZnO–ZnS composite in comparison with that of the ZnO template means a lifted Fermi level after vulcanization of the ZnO sheet template, and the more negative flat band potential of the ZnO sheet template after vulcanized modification means an enlarged degree of band bending in the material system [38]. Similarly, the M–S result of the g-C3N4-modified TiO2 heterostructure also exhibits the more negative flat band potential in the heterostructure with respect to that of the TiO2 template, and an enhanced charge separation efficiency is demonstrated in the g-C3N4-modified TiO2 heterostructure [41]. Furthermore, it has been shown that the conduction band energy (E CB) for the n-type semiconductor is more negative, i.e., about 0.1 eV than its flat band potential. [42]; therefore, the E CB of the pristine ZnO template herein can be evaluated as −0.6 eV vs NHE. Notably, for the construction of the ZnO/ZnS heterogeneous band structure for the ZS-1, the referenced M–S plot of a single ZnS phase is displayed in Figure 9(c), and the E CB of the ZnS is found to be roughly up to −0.89 eV vs NHE. Combined with the band gap energy obtained from the previous UV-vis results, the valence band energies (E VB) for the ZnO and ZnS are calculated to be 2.6 eV and 2.51 eV vs NHE, respectively, according to the equation E VB = E CB + E g.

Figure 9 Mott–Schottky plots of various products: (a) ZnO, (b) ZS-1, and (c) ZnS.
Figure 9

Mott–Schottky plots of various products: (a) ZnO, (b) ZS-1, and (c) ZnS.

Figure 10(a) presents the impressed potential-dependent degradation efficiency of the RhB solution by ZS-1 under 30 min irradiation. The PEC-degradation level of the RhB solution increased with increasing the impressed potential from 0 V to 0.5 V, and PEC-degradation efficiency of RhB solution reached a peak value of 58% at 0.5 V. Once the impressed potential exceeded 0.5 V, the degradation rate decreased (54%; 0.75 V). The result of Figure 10(a) demonstrates that a higher impressed potential (larger than 0.5 V) might result in reallocation of the space charge layers, further hindering the degradation efficiency [43]. Moreover, the ZS-1 was difficult to efficiently separate the photoinduced charges if the impressed voltage was lower than 0.5 V. Therefore, the optimal impressed potential for the ZnO–ZnS composite to the PEC-degrade RhB solution was chosen to be 0.5 V in this study. The photoelectrocatalytic performance of the ZnO template and various ZnO/ZnS composites toward the RhB solution is shown in Figure 10(b)–(e). The absorbance spectra intensity of the aqueous RhB solution decreased with irradiation duration for all the photoelectrocatalysts. In the PEC-degradation system, the absorbance peak of the RhB solution decreased during degradation without blue shift indicating the destruction of C═N, C═C, and C═O of the dye molecules due to the enhanced catalytic activity, and the final degradation products might consist of low-molecular-weight organic, CO2, H2O, etc. [43]. Figure 10(f) shows the RhB degradation efficiencies of ZnO, ZS-1, ZS-2, and ZS-3 are 57, 82, 72, and 43% under 60 min irradiation, respectively. Comparatively, the ZS-1 shows the highest degradation level toward the RhB solution among various control samples at the same given test convictions. Figure 10(g) presents the kinetic behaviors of the RhB solution degraded by ZnO and various ZnO–ZnS composites; the degradation rates of the RhB solution follow the pseudo-first-order reaction according to the simplified Langmuir–Hinshelwood model, −ln(C t /C 0) = kt, where C 0 is the initial concentration of the RhB solution, C t is the concentration of that at different intervals during the degradation process, and k is the reaction rate constant (min−1) [44]. The evaluated PEC-degradation rate constant of ZS-1 is 0.02493 min−1, which is 1.8, 1.2, and 2.8 times that of ZnO, ZS-2, and ZS-3, respectively. The PEC-degradation performance of ZS-1 and ZS-2 towards RhB solution is superior to that of the ZnO template, revealing the construction of ZnO–ZnS composite structure with suitable vulcanization conditions is beneficial to improve the PEC-degradation activity of the ZnO template. Furthermore, the recycling tests are conducted for the ZS-1 five times (Figure 10(h)). Notably, after five cycles, only a slight decrease of the photoelectrocatalytic activity is found, and 73% of RhB is degraded. The ZS-1 still maintains good photocatalyst activity (>70%) for RhB dye degradation herein, inferring that the prepared ZS-1 porous composite sheet catalyst is effective and reusable under sunlight irradiation.

Figure 10 (a) Absorbance spectra intensity variation of the RhB solution under different impressed voltages with the ZS-1. Absorbance spectra intensity variation of the RhB solution as a function of irradiation time with various products as photoelectrocatalysts: (b) ZnO, (c) ZS-1, (d) ZS-2, and (e) ZS-3. (f) C/C 0 vs irradiation time plot. (g) The reaction rate constants of various products. (h) Recycling PEC-degradation tests of the ZS-1 toward RhB solution.
Figure 10

(a) Absorbance spectra intensity variation of the RhB solution under different impressed voltages with the ZS-1. Absorbance spectra intensity variation of the RhB solution as a function of irradiation time with various products as photoelectrocatalysts: (b) ZnO, (c) ZS-1, (d) ZS-2, and (e) ZS-3. (f) C/C 0 vs irradiation time plot. (g) The reaction rate constants of various products. (h) Recycling PEC-degradation tests of the ZS-1 toward RhB solution.

Based on the experimental results, the possible photogenerated electron–hole pair transfer steps inside the ZnO/ZnS photoanode, and the degradation mechanism toward RhB dyes is shown in Figure 11(a). In the ZnO/ZnS composite system, the CB position of ZnO was located at −0.6 eV and that of ZnS was located approximately −0.89 eV from the M–S results. Figure 11(a) indicates that the constructed ZnO/ZnS system exhibited a staggered type-II band alignment configuration, which can lead to a spatial separation of the photoinduced electrons and holes. Notably, the oxidation ( ⋅ O 2 − / O 2 , ) and reduction (˙OH/H2O) potentials were −0.33 and +2.27 eV (vs NHE), respectively [2]. Excitation of electrons will take place in ZnO and ZnS simultaneously under irradiation. As the CB of ZnO is at a lower energy level than ZnS, the photogenerated electron will be transferred from CB of ZnS to the CB of ZnO, and further transported to the Pt counter electrode under an applied potential. By contrast, holes will migrate from the valence band (VB) of ZnO to the VB of ZnS, leading to the improved separation efficiency of photogenerated electron–hole pairs under the PEC system. The electrons at the Pt electrode and holes at the VB of ZnS would subsequently react with oxygen and water, respectively, to produce active superoxide and hydroxyl radicals for degradation processes. For further understanding of the photoelectrocatalytic mechanism, it is important to investigate the active species formed during the photoelectrocatalytic process toward the RhB solution. Benzoquinone (BQ), edentate disodium (EDTA), and tert-butyl alcohol (t-BuOH) were employed to scavenge the superoxide radicals ( ⋅ O 2 − ), the hole (h+), and hydroxyl radicals (˙OH), respectively, herein. As shown in Figure 11(b), the photoelectrocatalytic activity of ZS-1 has been significantly decreased when BQ is added, indicating the superoxide radicals ( ⋅ O 2 − ) are the main reactive species in the photodegradation process. Comparatively, when introducing EDTA and t-BuOH, the degradation has been decreased for a lower degree, suggesting that h+ and ˙OH also participate in the photocatalytic reaction for the ZS-1 toward RhB solution, but the effect is smaller than that of the ⋅ O 2 − species. Based on the above results, a schematic diagram of the possible degradation mechanisms of the photoinduced charges in the ZS-1 heterostructure is also constructed in Figure 11(a). The type II alignment of the ZnO–ZnS junction promoted the electron flowing from CBZnS to CBZnO and further transport to the Pt counter electrode, and then the O2 accepted the electrons to generate ⋅ O 2 − . Furthermore, VBZnS (2.51 eV) was more positive than the highest unoccupied molecular orbital (HOMO) of RhB (1.6 eV), the holes at the VB of ZnS can directly degrade RhB molecules and/or reaction with H2O molecules for ˙OH radicals to degrade RhB molecules. Similarly, because of a more positive potential than the HOMO of RhB, photoinduced holes at the VB of Bi2WO6 in WO3/Bi2WO6 heterostructures can directly react with RhB molecules or react with H2O to generate ˙OH radicals to degrade RhB dyes effectively. [45]. As the applied potential accelerates the separation and transfer efficiency of photoinduced charges, it results in high PEC degradation efficiency of ZS-1. We put forward the possible action trails for reactive species as follows:

(1) ZnO + h v → ZnO ( e − + h + ) ,

(2) ZnS + h v → ZnS ( e − + h + ) ,

(3) e − ( Pt ) + O 2 → ⋅ O 2 − ,

(4) h + ( VB ZnS ) + H 2 O → ⋅ OH + H + ,

(5) ⋅ O 2 − , h + , ⋅ OH + RhB → CO 2 + H 2 O .

The aforementioned potential enhanced photoinduced charge separation is similar to the PEC-degradation of In2O3–ZnO composites with a type II band alignment toward the MB solution [46]. The electron drift and hole capture in Type II band alignment will suppress the recombination of photoinduced electron–hole pairs. Meanwhile, the applied voltage will rapidly prompt the photogenerated electrons to move to the external circuit rapidly, which tremendously reduces the recombination of electron–hole pairs. The improved photoelectrocatalytic activity of ZS-1 and ZS-2 composites with suitable ZnS/ZnO phase ratios than that of the pristine ZnO template herein was mainly ascribed to the formation of heterojunctions, which improved the absorption efficiency of light and inhibited the recombination of the photogenerated electron–hole pairs and the apparent synergetic effect between photo- and electrocatalysis, which facilitated charge generation, separation, and transfer. It has been shown that the comparative component ratio in the heterostructures is highly associated with their photocatalytic performances [46]. Moreover, the porous structure of the composites because of the high specific surface area is also beneficial to the photocatalytic activity [47]. Based on the aforementioned points, the porous structure and the optimal ZnS/ZnO phase ratio in the ZS-1 sheet impacted the superior photoelectrocatalytic performance toward degrading RhB dyes with respect to other ZnO–ZnS composites in this study. Similar porous structure and composition ratio effects dominating the optimal photocatalytic activity have also been demonstrated in ZnS–SnS2 porous nanosheets [47].

Figure 11 (a) The possible band structures and PEC-degradation mechanism of the ZS-1 toward RhB solution. (b) Scavenger tests of the RhB solution containing ZS-1.
Figure 11

(a) The possible band structures and PEC-degradation mechanism of the ZS-1 toward RhB solution. (b) Scavenger tests of the RhB solution containing ZS-1.

4 Conclusion

The sheet-like ZnO–ZnS composites were successfully synthesized by the hydrothermal vulcanization method of porous ZnO sheet templates. The microstructure and composition analyses results reveal that the sulfur precursor concentration affected the ZnO/ZnS phase ratio and surface morphology of the as-synthesized ZnO–ZnS sheet composites. Compared with pristine ZnO, the ZnO–ZnS composites with the S/O atomic composition ratios of 0.61 and 0.85 substantially reduced the recombination rate of photogenerated electron–hole pairs by enhanced charge separation. By contrast, the ZnO–ZnS composite with the higher S/O atomic composition ratio of 3.63 decreased the photoactivity. The suitable ZnO/ZnS phase ratio and the porous surface feature made the ZS-1 porous sheet composite exhibit superior photoactivity among various control samples. In this study, the ZS-1 photoanode had a high photocurrent density of 1.22 mA/cm2 at 0.5 V (vs Ag/AgCl), and highly efficient PEC-degradation ability toward RhB solution to over 80% at 0.5 V. The integration of the hydrothermally derived porous ZnO sheet template with a vulcanization process to control surface porous features and the ZnO/ZnS phase ratio by varying sulfur precursor concentrations is a promising approach to design the ZnS–ZnO sheet composite with various degrees of photoactive performances for photoelectrocatalyst applications.

  1. Funding information: This research was funded by the Ministry of Science and Technology of Taiwan, Grant No. MOST 108-2221-E-019-034-MY3.

  2. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Conflict of interest: The authors state no conflict of interest.

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Received: 2021-11-10
Revised: 2022-01-05
Accepted: 2022-02-17
Published Online: 2022-03-14

© 2022 Yuan-Chang Liang and Chia-Hung Huang, published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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  59. Mechanical properties and microstructure of nano-strengthened recycled aggregate concrete
  60. Glucose-responsive nanogels efficiently maintain the stability and activity of therapeutic enzymes
  61. Tunning matrix rheology and mechanical performance of ultra-high performance concrete using cellulose nanofibers
  62. Flexible MXene/copper/cellulose nanofiber heat spreader films with enhanced thermal conductivity
  63. 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
  64. 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
  65. An implication of magnetic dipole in Carreau Yasuda liquid influenced by engine oil using ternary hybrid nanomaterial
  66. Robust synthesis of a composite phase of copper vanadium oxide with enhanced performance for durable aqueous Zn-ion batteries
  67. Tunning self-assembled phases of bovine serum albumin via hydrothermal process to synthesize novel functional hydrogel for skin protection against UVB
  68. A comparative experimental study on damping properties of epoxy nanocomposite beams reinforced with carbon nanotubes and graphene nanoplatelets
  69. Lightweight and hydrophobic Ni/GO/PVA composite aerogels for ultrahigh performance electromagnetic interference shielding
  70. Research on the auxetic behavior and mechanical properties of periodically rotating graphene nanostructures
  71. Repairing performances of novel cement mortar modified with graphene oxide and polyacrylate polymer
  72. Closed-loop recycling and fabrication of hydrophilic CNT films with high performance
  73. Design of thin-film configuration of SnO2–Ag2O composites for NO2 gas-sensing applications
  74. Study on stress distribution of SiC/Al composites based on microstructure models with microns and nanoparticles
  75. PVDF green nanofibers as potential carriers for improving self-healing and mechanical properties of carbon fiber/epoxy prepregs
  76. Osteogenesis capability of three-dimensionally printed poly(lactic acid)-halloysite nanotube scaffolds containing strontium ranelate
  77. Silver nanoparticles induce mitochondria-dependent apoptosis and late non-canonical autophagy in HT-29 colon cancer cells
  78. Preparation and bonding mechanisms of polymer/metal hybrid composite by nano molding technology
  79. Damage self-sensing and strain monitoring of glass-reinforced epoxy composite impregnated with graphene nanoplatelet and multiwalled carbon nanotubes
  80. Thermal analysis characterisation of solar-powered ship using Oldroyd hybrid nanofluids in parabolic trough solar collector: An optimal thermal application
  81. Pyrene-functionalized halloysite nanotubes for simultaneously detecting and separating Hg(ii) in aqueous media: A comprehensive comparison on interparticle and intraparticle excimers
  82. Fabrication of self-assembly CNT flexible film and its piezoresistive sensing behaviors
  83. Thermal valuation and entropy inspection of second-grade nanoscale fluid flow over a stretching surface by applying Koo–Kleinstreuer–Li relation
  84. Mechanical properties and microstructure of nano-SiO2 and basalt-fiber-reinforced recycled aggregate concrete
  85. Characterization and tribology performance of polyaniline-coated nanodiamond lubricant additives
  86. Combined impact of Marangoni convection and thermophoretic particle deposition on chemically reactive transport of nanofluid flow over a stretching surface
  87. Spark plasma extrusion of binder free hydroxyapatite powder
  88. An investigation on thermo-mechanical performance of graphene-oxide-reinforced shape memory polymer
  89. 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
  90. Design selection for a hemispherical dimple core sandwich panel using hybrid multi-criteria decision-making methods
  91. Improving tensile strength and impact toughness of plasticized poly(lactic acid) biocomposites by incorporating nanofibrillated cellulose
  92. Green synthesis of spinel copper ferrite (CuFe2O4) nanoparticles and their toxicity
  93. The effect of TaC and NbC hybrid and mono-nanoparticles on AA2024 nanocomposites: Microstructure, strengthening, and artificial aging
  94. Excited-state geometry relaxation of pyrene-modified cellulose nanocrystals under UV-light excitation for detecting Fe3+
  95. Effect of CNTs and MEA on the creep of face-slab concrete at an early age
  96. Effect of deformation conditions on compression phase transformation of AZ31
  97. Application of MXene as a new generation of highly conductive coating materials for electromembrane-surrounded solid-phase microextraction
  98. A comparative study of the elasto-plastic properties for ceramic nanocomposites filled by graphene or graphene oxide nanoplates
  99. Encapsulation strategies for improving the biological behavior of CdS@ZIF-8 nanocomposites
  100. Biosynthesis of ZnO NPs from pumpkin seeds’ extract and elucidation of its anticancer potential against breast cancer
  101. Preliminary trials of the gold nanoparticles conjugated chrysin: An assessment of anti-oxidant, anti-microbial, and in vitro cytotoxic activities of a nanoformulated flavonoid
  102. Effect of micron-scale pores increased by nano-SiO2 sol modification on the strength of cement mortar
  103. Fractional simulations for thermal flow of hybrid nanofluid with aluminum oxide and titanium oxide nanoparticles with water and blood base fluids
  104. The effect of graphene nano-powder on the viscosity of water: An experimental study and artificial neural network modeling
  105. Development of a novel heat- and shear-resistant nano-silica gelling agent
  106. Characterization, biocompatibility and in vivo of nominal MnO2-containing wollastonite glass-ceramic
  107. Entropy production simulation of second-grade magnetic nanomaterials flowing across an expanding surface with viscidness dissipative flux
  108. Enhancement in structural, morphological, and optical properties of copper oxide for optoelectronic device applications
  109. Aptamer-functionalized chitosan-coated gold nanoparticle complex as a suitable targeted drug carrier for improved breast cancer treatment
  110. Performance and overall evaluation of nano-alumina-modified asphalt mixture
  111. Analysis of pure nanofluid (GO/engine oil) and hybrid nanofluid (GO–Fe3O4/engine oil): Novel thermal and magnetic features
  112. Synthesis of Ag@AgCl modified anatase/rutile/brookite mixed phase TiO2 and their photocatalytic property
  113. Mechanisms and influential variables on the abrasion resistance hydraulic concrete
  114. Synergistic reinforcement mechanism of basalt fiber/cellulose nanocrystals/polypropylene composites
  115. Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
  116. Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
  117. Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
  118. Effects of nano-ZrSi2 on thermal stability of phenolic resin and thermal reusability of quartz–phenolic composites
  119. Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
  120. Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
  121. Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
  122. Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
  123. Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
  124. Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
  125. Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
  126. Mechanisms of the improved stiffness of flexible polymers under impact loading
  127. Anticancer potential of gold nanoparticles (AuNPs) using a battery of in vitro tests
  128. Review Articles
  129. Proposed approaches for coronaviruses elimination from wastewater: Membrane techniques and nanotechnology solutions
  130. Application of Pickering emulsion in oil drilling and production
  131. The contribution of microfluidics to the fight against tuberculosis
  132. Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
  133. Synthesis and encapsulation of iron oxide nanorods for application in magnetic hyperthermia and photothermal therapy
  134. Contemporary nano-architectured drugs and leads for ανβ3 integrin-based chemotherapy: Rationale and retrospect
  135. State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
  136. Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
  137. A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
  138. Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
  139. Advances in ZnO: Manipulation of defects for enhancing their technological potentials
  140. Efficacious nanomedicine track toward combating COVID-19
  141. A review of the design, processes, and properties of Mg-based composites
  142. Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
  143. Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
  144. Recent progress and challenges in plasmonic nanomaterials
  145. Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
  146. Electronic noses based on metal oxide nanowires: A review
  147. Framework materials for supercapacitors
  148. An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
  149. Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
  150. Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
  151. A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
  152. Recent advances in the preparation of PVDF-based piezoelectric materials
  153. Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
  154. Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
  155. Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
  156. Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
  157. Nanotechnology application on bamboo materials: A review
  158. Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
  159. Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
  160. 3D printing customized design of human bone tissue implant and its application
  161. Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
  162. A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
  163. Nanotechnology interventions as a putative tool for the treatment of dental afflictions
  164. Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
  165. A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
  166. Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
  167. Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
  168. Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
  169. Molecular dynamics application of cocrystal energetic materials: A review
  170. Synthesis and application of nanometer hydroxyapatite in biomedicine
  171. Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
  172. Biological applications of ternary quantum dots: A review
  173. Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
  174. Application of antibacterial nanoparticles in orthodontic materials
  175. Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
  176. Nanozymes – A route to overcome microbial resistance: A viewpoint
  177. Recent developments and applications of smart nanoparticles in biomedicine
  178. Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
  179. Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
  180. Diamond-like carbon films for tribological modification of rubber
  181. Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
  182. Recent research progress and advanced applications of silica/polymer nanocomposites
  183. Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
  184. Recent advances in perovskites-based optoelectronics
  185. Biogenic synthesis of palladium nanoparticles: New production methods and applications
  186. A comprehensive review of nanofluids with fractional derivatives: Modeling and application
  187. Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
  188. Electrohydrodynamic printing for demanding devices: A review of processing and applications
  189. Rapid Communications
  190. Structural material with designed thermal twist for a simple actuation
  191. Recent advances in photothermal materials for solar-driven crude oil adsorption
https://doi.org/10.1515/ntrev-2022-0076
Keywords for this article
sheet composite; microstructure; photoactive performance
Creative Commons
BY 4.0

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  115. Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
  116. Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
  117. Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
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  119. Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
  120. Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
  121. Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
  122. Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
  123. Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
  124. Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
  125. Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
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  128. Review Articles
  129. Proposed approaches for coronaviruses elimination from wastewater: Membrane techniques and nanotechnology solutions
  130. Application of Pickering emulsion in oil drilling and production
  131. The contribution of microfluidics to the fight against tuberculosis
  132. Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
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  135. State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
  136. Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
  137. A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
  138. Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
  139. Advances in ZnO: Manipulation of defects for enhancing their technological potentials
  140. Efficacious nanomedicine track toward combating COVID-19
  141. A review of the design, processes, and properties of Mg-based composites
  142. Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
  143. Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
  144. Recent progress and challenges in plasmonic nanomaterials
  145. Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
  146. Electronic noses based on metal oxide nanowires: A review
  147. Framework materials for supercapacitors
  148. An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
  149. Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
  150. Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
  151. A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
  152. Recent advances in the preparation of PVDF-based piezoelectric materials
  153. Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
  154. Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
  155. Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
  156. Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
  157. Nanotechnology application on bamboo materials: A review
  158. Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
  159. Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
  160. 3D printing customized design of human bone tissue implant and its application
  161. Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
  162. A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
  163. Nanotechnology interventions as a putative tool for the treatment of dental afflictions
  164. Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
  165. A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
  166. Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
  167. Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
  168. Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
  169. Molecular dynamics application of cocrystal energetic materials: A review
  170. Synthesis and application of nanometer hydroxyapatite in biomedicine
  171. Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
  172. Biological applications of ternary quantum dots: A review
  173. Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
  174. Application of antibacterial nanoparticles in orthodontic materials
  175. Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
  176. Nanozymes – A route to overcome microbial resistance: A viewpoint
  177. Recent developments and applications of smart nanoparticles in biomedicine
  178. Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
  179. Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
  180. Diamond-like carbon films for tribological modification of rubber
  181. Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
  182. Recent research progress and advanced applications of silica/polymer nanocomposites
  183. Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
  184. Recent advances in perovskites-based optoelectronics
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