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Heteropolyacid-loaded MOF-derived mesoporous zirconia catalyst for chemical degradation of rhodamine B

  • Jialu Wang EMAIL logo , Rongfei Yu , Zhenying Li , Fen Yang , Linmin Luo , Dandan Wang , Huan Cheng , Yutao Zhang EMAIL logo and Qiuyun Zhang EMAIL logo
Published/Copyright: April 18, 2023
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Green Processing and Synthesis
From the journal Green Processing and Synthesis Volume 12 Issue 1

Abstract

In this article, silicotungstic acid (STA)-loaded metal–organic framework (MOF)-derived composites (C-STA@ZrO2) were successfully synthesized by simple strategies. X-ray diffraction, Fourier transform infrared, scanning electron microscopy, energy-dispersive X-ray, N2 physisorption, UV-vis diffuse reflection spectroscopy, and X-ray photoelectron spectroscopy techniques were used to characterize the as-obtained composites. Intriguingly, C-STA@ZrO2 exhibits excellent photocatalytic performance, and rhodamine B (RhB) (40 mg·L−1) in water can be degraded to 93.9% after 120 min of irradiation. Moreover, various catalysts, catalyst dosage, and dye concentrations on RhB degradation were evaluated. Besides, the reusability of C-STA@ZrO2 was also investigated. This work may provide a new and significant guideline for exploring excellent performance of MOF-derived hybrid material for wastewater purification.

Keywords: metal–organic framework; silicotungstic acid; photocatalysis; rhodamine B; photodegradation

1 Introduction

With the rapid development of the printing and dyeing industries, the demand for organic dyes is growing rapidly [1]. However, these organic dyes are inevitably discharged into water, which can increase the extent of environmental pollution and disturb ecosystems because of their non-biodegradability and high toxicity [2,3]. To solve these problems, various methods (e.g., physical adsorption, chemical oxidation, and biological treatment) have been studied to remove the dye-contaminated water [4,5,6,7,8,9]. Among these techniques, the photocatalysis technique has been highlighted as one of the most promising methods for wastewater remediation [10]. During the photocatalytic reaction, many photocatalysts (e.g., metal oxides, graphitic carbon nitride, and zeolites) have been widely studied [11].

Recently, heteropolyacids are receiving considerable attention in the photocatalysis field, such as silicotungstic acid (STA), phosphomolybdic acid, and tungstophosphoric acid, because of their high catalytic, unique redox properties, and electron trapping capacity; especially, the unoccupied W 5d states of the Keggin STA unit can be used as an electron trap [12,13]. Unfortunately, the practical engineering application of heteropolyacids is limited due to their high solubility in polar solvents and low surface area [14]. Therefore, several modification techniques (e.g., supporting and doping) have been investigated, aiming to solve this problem [15]. Among them, loading heteropolyacids into porous substances with high surface area is one of the most promising strategies.

Metal–organic framework (MOF), constructed from metal ions/clusters and organic linkers, has been widely used in various fields owing to its clear porosity, large specific surface areas, and tailorability [16,17,18,19]. In particular, Zr-base MOF (e.g., UiO-66) has demonstrated excellent performance in a variety of photocatalysis reactions, due to various features, such as high defect tolerance and high hydrothermal stability [20,21]. More recently, through a simple heat treatment process, MOF can be transformed into hierarchically porous metal oxides, which is beneficial to enhance interaction between metal oxides and active components [22,23,24]. Thus, MOF-derived metal oxide skeletons are an ideal candidate for loading heteropolyacids. In this study, UiO-66-derived zirconia (ZrO2) skeletons as support-loaded STA hybrids (C-STA@ZrO2) were synthesized via a one-pot hydrothermal process followed by heat treatment strategy for visible light degradation of rhodamine B (RhB) dye. The hybrids were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR), scanning electron microscopy (SEM), energy-dispersive X-ray (EDX), N2 physisorption, UV-vis diffuse reflection spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), etc. Furthermore, the stability of C-STA@ZrO2 and the possible degradation mechanism were also explored.

2 Materials and methods

2.1 Reagents

Zirconium(iv) chloride (ZrCl4), terephthalic acid (H2BDC), silicotungstic acid (STA, H4SiW12O40·nH2O), N,N-dimethylformamide (DMF), absolute ethanol, RhB, congo red (CR), acridine orange (AO), and methylene blue (MB) were obtained from Sigma-Aldrich. All reagents were of analytical grade and were used directly without any further purification.

2.2 Synthesis

STA-loaded MOF-derived ZrO2 was prepared through a sample way. Briefly, H2BDC (2 mmol, 0.3323 g), ZrCl4 (1 mmol, 0.233 g), and STA (0.3 g) were dissolved in 18 mL ethanol and kept for 10 min under ultrasound conditions and subsequently stirred for 60 min at ambient temperature. Then, the aforementioned mixture was transferred into an autoclave and heated at 150°C for 6 h. After the autoclave was cooled, the resulting precipitate was centrifuged and washed with DMF and deionized water three times. Finally, the obtained samples were dried and annealed at 350°C for 2 h with the heating rate of 5°C·min−1, and the hybrid material was marked as C-STA@ZrO2. Besides, the synthesis route of C-STA@ZrO2 composite is presented in Scheme 1. In addition, C-ZrO2 without adding STA was fabricated using a similar process.

Scheme 1 Synthesis route of C-STA@ZrO2 composite.
Scheme 1

Synthesis route of C-STA@ZrO2 composite.

2.3 Characterization techniques

The XRD patterns were identified by D8 ADVANCE (Germany) using CuKα (1.5406 Å) radiation in the 2θ range of 5–65°. FTIR spectra were measured to determine the chemical features of the samples on a PerkinElmer spectrum 100 using KBr pellet technology (4,000–400 cm−1). The particle sizes and morphologies of the catalysts were observed using SEM (Hitachi S-4800, Japan), and element distribution was obtained on EDX. The surface area and particle sizes of the as-obtained samples were measured by N2 adsorption and desorption isotherms using a Quantachrome Quadrasorb EVO apparatus (Quantachrome Instruments, Boynton Beach, USA). UV-vis diffuse reflectance spectroscopy of the as-obtained samples was recorded through UV-vis spectrophotometer (Shimadzu, UV-3600 PLUS, Japan).

2.4 Photochemical reactions

The photocatalytic performance of the as-obtained catalysts toward organic pollutant degradation was evaluated under visible light irradiation at room temperature. Typically, 0.05 g catalyst was mixed with 50 mL of 40 mg·L−1 RhB aqueous solution. Before photodegradation, the solution was stirred in the dark for 30 min to ensure the adsorption equilibrium. Then, the resulting solution was irradiated with a 300 W xenon arc lamp for 2 h. At specific time intervals, a sample of 3–4 mL was taken out, centrifuged, and analyzed by a UV-5200 PC spectrophotometer at the characteristic wavelength. To evaluate the reusability, the catalyst was separated by centrifugation after each use, washed with DMF, and vacuum-dried overnight for the next photodegradation. Moreover, the photodegradation rate of RhB could be calculated by the following equation:

(1) R ( % ) = ( 1 − C / C 0 ) × 100 % ,

where C 0 is the initial concentration of RhB and C is the concentration of RhB after “t” minutes illumination, respectively.

3 Results and discussion

3.1 Characterization

The XRD diffractograms of STA, UiO-66C-ZrO2, STA@UiO-66, and C-STA@ZrO2 catalysts are shown in Figures A1 and A2 (in Appendix). According to Figure A2, UiO-66 has two distinct characteristic peaks at 7.3° and 8.5° corresponding to crystal planes (111) and (200), indicating that UiO-66 is successfully synthesized [25]. As shown in Figure A1, it is worth noting that the XRD diffraction peaks of C-ZrO2 and STA@UiO-66 catalysts are similar to that of UiO-66, which is attributed to the similar structural features. It also indicates that the crystal structure of UiO-66 is well maintained during the pyrolysis process and the introduction of STA. As STA@UiO-66 is calcined at 350°C, C-STA@ZrO2 shows the diffraction peak position similar to the C-ZrO2 catalyst, indicating that the C-ZrO2 and C-STA@ZrO2 have the same structure. However, compared to C-ZrO2, the peak intensities were slightly weaker for the C-STA@ZrO2 sample, which may be due to the interaction between the generation of zirconia (ZrO2) and STA [26]. In addition, no evident STA peaks were observed in the STA@UiO-66 and C-STA@ZrO2 hybrids; it was possible due to the STA being well dispersed on the framework structure [27]. According to the XRD analysis results, the successful synthesis of STA-loaded MOF-derived ZrO2 catalyst was performed.

The FTIR spectra patterns of the STA, UiO-66, C-ZrO2, STA@UiO-66, and C-STA@ZrO2 catalysts are presented in Figure 1. The FTIR spectra of STA have four distinct absorption peaks at 804, 884, 927, and 980 cm−1, corresponding to the Keggin structure of STA. Notably, all peaks of UiO-66 that appeared in the FTIR spectra are well agreed with those previously reported [28], which confirmed that UiO-66 had been successfully synthesized. Compared to UiO-66, the FTIR spectra of C-ZrO2 and C-STA@ZrO2 are similar to that of UiO-66, but the intensity of all bands decreases greatly after the pyrolysis, which may be due to the partial decomposition of the organic ligand and the generation of ZrO2. Moreover, the characteristic absorption peaks of STA are found in the STA@UiO-66 and C-STA@ZrO2 hybrids, which is evident that the STA groups were attached to UiO-66 and the skeleton structure of STA was not decomposed during pyrolysis process, and this is consistent with XRD results.

Figure 1 FTIR spectra of obtained photocatalysts.
Figure 1

FTIR spectra of obtained photocatalysts.

SEM analysis in Figure 2 showed the morphological features of the synthesized UiO-66, C-ZrO2, and C-STA@ZrO2 catalysts. As shown in Figure 2a, UiO-66 exhibits spherical particles with aggregation nature. Compared to morphology of UiO-66 before and after calcination, sintering and the shrinkage of particles occurred, resulting in the formation of sphere-shaped particles with a size of about 200 nm for C-ZrO2 (Figure 2b). When the STA is introduced, it can be seen from Figure 2c and d that C-STA@ZrO2 catalyst was messy and rough with an irregular dimensional nearly sphere-like shaped particles, and the obvious pore structure and aggregation could be observed. This phenomenon may be explained by the presence of strong interaction between STA and ZrO2 after thermal transition process, which may cause an important effect on the surface morphology. Simultaneously, it is also noted that the presence of pore structure can decrease the recombination rate of electron–hole pairs and is further beneficial for photocatalysis applications [29]. Besides, the elements of the prepared C-STA@ZrO2 catalyst were verified by EDS, and it can be seen from Figure 2e that Zr and W elements existed in the sample, suggesting the successful preparation of the C-STA@ZrO2 composite.

Figure 2 SEM micrographs of UiO-66 (a), C-ZrO2 (b), C-STA@ZrO2 (c and d), and (e) the corresponding Zr and W elemental mapping images.
Figure 2

SEM micrographs of UiO-66 (a), C-ZrO2 (b), C-STA@ZrO2 (c and d), and (e) the corresponding Zr and W elemental mapping images.

The optical properties of the synthesized C-ZrO2 and C-STA@ZrO2 catalysts were assessed by UV-vis DRS analysis. As shown in Figure 3a, C-ZrO2 and C-STA@ZrO2 exhibited strong absorption responses in the visible light region (200–800 nm). The maximum absorption band edges of C-ZrO2 and C-STA@ZrO2 are about 338 and 440 nm, respectively, illustrating that the impregnation of STA could effectively improve the optical response range of C-ZrO2. In addition, the optical bandgap of catalyst can be estimated from the Tauc plot method [30]. As illustrated in Figure 3b, the bandgap values (E g) of the materials were calculated to be 3.93 and 3.11 eV for C-ZrO2 and C-STA@ZrO2, respectively. It could be distinctly observed that the C-STA@ZrO2 displayed an obvious red shift compared with C-ZrO2, revealing the interaction between STA and ZrO2 in the C-STA@ZrO2 heterostructure [31], and it matched the SEM results. Moreover, the aforementioned results also revealed that the loading of STA would narrow the bandgap of C-ZrO2 and enhance visible light absorption.

Figure 3 (a) UV-Vis absorption spectra and (b) the Tauc plots of C-ZrO2 and C-STA@ZrO2 catalysts; (c) N2 physisorption isotherm and (d) BJH pore-size distribution of C-STA@ZrO2 catalyst.
Figure 3

(a) UV-Vis absorption spectra and (b) the Tauc plots of C-ZrO2 and C-STA@ZrO2 catalysts; (c) N2 physisorption isotherm and (d) BJH pore-size distribution of C-STA@ZrO2 catalyst.

Figure 3c and d displays the N2 adsorption–desorption isotherms and the BJH pore-size distribution pattern of C-STA@ZrO2 catalyst. Obviously, the C-STA@ZrO2 has a type-IV isotherm model, and correspondingly, the BJH pore-size distribution exhibited the presence of mesopores in the composite. According to previous studies [32], STA@UiO-66 has a larger BET surface area (>700 m2·g−1). When the STA@UiO-66 was calcined, the UiO-66 structure shrinks and collapses, and the produced ZrO2 formed, resulting in the decreased BET surface area (390.5 m2·g−1). In addition, pore volume and pore diameter of the C-STA@ZrO2 catalyst were 0.215 cm3·g−1 and 2.2 nm, respectively. The aforementioned findings revealed that C-STA@ZrO2 still possessed mesopore and high BET surface area and pore volume, which is conducive to reducing transfer resistance and enhancing adsorption reactant molecules [33]. Thus, it is supposed that C-STA@ZrO2 has a better photocatalytic activity in this work.

Also, the XPS spectra of C-STA@ZrO2 were found, and the results are illustrated in Figure 4. It can be seen from Figure 4a that the C-STA@ZrO2 catalyst possesses characteristic peaks of O, C, Zr, and W. As shown in Figure 4b, the O 1s peaks of the catalyst are located at 530.1, 531.8, and 533.2 eV, corresponding to W–O, surface hydroxyl oxygen, and weakly absorbed oxygen, respectively [34]. The Zr 3d XPS spectrum in Figure 4c simulated the two peaks around 182.8 and 185.1 eV that are attributed to Zr 3d5/2 and Zr 3d3/2, which can prove the existence of Zr4+ As shown in Figure 4d, the peaks labeled by 35.6 and 37.7 eV could be assigned to W 4f7/2 and W 4f5/2 representing the presence of W6+ [35]. Other peaks at 30–32 eV can be observed, which are attributed to the partial decomposition of STA and the formation of an oxide state, and a similar behavior was observed by Xu et al. [36]. The aforementioned results confirmed that the C-STA@ZrO2 composite has been successfully synthesized.

Figure 4 XPS spectrum of the C-STA@ZrO2: (a) survey spectrum, (b) O 1s, (c) Zr 3d, and (d) W 4f.
Figure 4

XPS spectrum of the C-STA@ZrO2: (a) survey spectrum, (b) O 1s, (c) Zr 3d, and (d) W 4f.

3.2 Photocatalytic activity of synthesized catalysts

The UV absorption spectra during the degradation process are displayed in Figure 5a. It is clear that the absorbance peak intensity of RhB at 554 nm gradually weakened as time increased and the absorption peak is blue-shifted, which can be explained by the step-by-step deethylation process of RhB in the photocatalytic system [37]. Moreover, the photocatalytic performances of C-ZrO2 and C-STA@ZrO2 catalysts were studied (Figure 5b). As can be seen in Figure 5b, RhB was hardly decomposed by direct photolysis, and it was also not removed with C-STA@ZrO2 catalyst under the dark. In addition, it can be seen that C-STA@ZrO2 has a higher degradation activity than C-ZrO2 under visible-light irradiation, and the degradation rate of RhB (40 mg·L−1) by C-ZrO2 and C-STA@ZrO2 catalysts is approximately 58.2% and 93.9% in 120 min, respectively. As shown in Figure 5c, it is found that the linear relationship between In(C 0/C) and reaction time for C-ZrO2 and C-STA@ZrO2 catalysts follows the first-order kinetics. Furthermore, the average kinetic rate constants (k) of C-ZrO2 and C-STA@ZrO2 are 0.0072 and 0.0231 min−1, respectively, indicating that the k value of C-STA@ZrO2 is 3.2 times higher than that of C-ZrO2. The good catalytic performance of C-STA@ZrO2 catalyst is ascribed to reduce the bandgap of material, the synergistic effects between STA and C-ZrO2 leading to enhanced photon absorption after the loading of STA.

Figure 5 (a) UV-Vis absorption curves of RhB at different times in the presence of C-STA@ZrO2 catalyst; (b) photocatalytic performance of various catalysts (conditions: catalyst loading = 1.0 g·L−1; initial RhB concentration = 40 mg·L−1). (c) In(C o/C) vs time for various catalysts for the degradation of RhB dye.
Figure 5

(a) UV-Vis absorption curves of RhB at different times in the presence of C-STA@ZrO2 catalyst; (b) photocatalytic performance of various catalysts (conditions: catalyst loading = 1.0 g·L−1; initial RhB concentration = 40 mg·L−1). (c) In(C o/C) vs time for various catalysts for the degradation of RhB dye.

3.3 Influential factors on the photodegradation of RhB

Figure 6a depicts the effect of catalyst amount on the photodegradation of RhB. From Figure 6a, the improvement in degradation rate was observed with the increase in C-STA@ZrO2 amount, and the degradation rate was found to be 93.9% for C-STA@ZrO2 concentrations of 1.0 g·L−1. This result was attributed to the fact that increasing the catalyst is responsible for the generation of more activated radicals toward RhB degradation [38]. When the amount of the catalyst is further increased, the photocatalytic performance levels off, and this may be attributed to the light reflection and the shielding effect [39]. Therefore, C-STA@ZrO2 concentrations of 1.0 g·L−1 was selected. Additionally, the effect of initial concentrations of RhB was also examined, as shown in Figure 6b. These experimental results have shown that the photocatalytic rate of C-STA@ZrO2 decreased from 93.9% to 74.4% as the RhB dye concentration was increased from 40 to 60 mg·L−1 in 120 min. This is possible because the active sites on the surface of C-STA@ZrO2 are available to a particular limit [40]. Therefore, the degradation rate decreases with the increase in the initial concentrations of RhB, and the initial RhB concentrations of 40 mg·L−1 are selected for photodegradation.

Figure 6 (a) Effect of amount of the C-STA@ZrO2 catalyst on the photocatalytic degradation of RhB dye (40 mg·L−1). (b) Photocatalytic degradation of RhB dye at various initial dye concentrations in the presence of C-STA@ZrO2 (1.0 g·L−1) catalyst. (c) Photocatalytic degradation of different dyes in the presence of C-STA@ZrO2 (1.0 g·L−1) catalyst. (d) Degradation of RhB dye after three cycles in the presence of C-STA@ZrO2 catalyst (conditions: catalyst loading = 1.0 g·L−1; initial RhB concentration = 40 mg·L−1).
Figure 6

(a) Effect of amount of the C-STA@ZrO2 catalyst on the photocatalytic degradation of RhB dye (40 mg·L−1). (b) Photocatalytic degradation of RhB dye at various initial dye concentrations in the presence of C-STA@ZrO2 (1.0 g·L−1) catalyst. (c) Photocatalytic degradation of different dyes in the presence of C-STA@ZrO2 (1.0 g·L−1) catalyst. (d) Degradation of RhB dye after three cycles in the presence of C-STA@ZrO2 catalyst (conditions: catalyst loading = 1.0 g·L−1; initial RhB concentration = 40 mg·L−1).

3.4 Photocatalytic degradation of various dyes

Figure 6c shows the photodegradation of different dyes in the C-STA@ZrO2 system. Clearly, the degradation rates of CR (40 mg·L−1), AO (40 mg·L−1), MB (20 mg·L−1), and RhB (40 mg·L−1) in the C-STA@ZrO2 system were 66.6%, 97.4%, 95.8%, and 93.9% after 120 min, respectively. These results suggest that the as-designed C-STA@ZrO2 system can effectively and photocatalytically degrade organic dyes from wastewater.

3.5 Cycling stability

To evaluate the photocatalytic stability of the C-STA@ZrO2 catalyst, cycle experiments were performed. After every cycle, the catalyst was separated, washed, and dried for next use. As shown in Figure 6d, it shows that the degradation rate of the C-STA@ZrO2 catalyst decreased by only 32.8% after three consecutive experiments. Besides, the structures of C-STA@ZrO2 before and after three cycles are also presented in Figure A1 and Figure 1. The results reveal that the characteristic XRD and FTIR peaks of the C-STA@ZrO2 after three cycles were similar to the peaks for the original catalyst, suggesting that the structure of C-STA@ZrO2 was relatively stable. However, this reduction in catalytic performance might be because of the partial loss of the photocatalyst during the recovery process [41]. Based on the aforementioned discussion, the C-STA@ZrO2 composite has a relatively good photostability.

3.6 Possible photocatalytic mechanisms

The possible photocatalytic degradation mechanism of RhB by the C-STA@ZrO2 catalyst under visible light irradiation is shown in Scheme 2. The bandgap values (E g) of C-ZrO2 and C-STA@ZrO2 were estimated by the Tauc plot method in combination with Figure 3b, which were 3.93 and 3.11 eV, respectively, which could be that the loading of STA will induce an intermediate energy level in the bandgap region of C-ZrO2, and this intermediate energy level allows electrons to move toward it, making the bandgap smaller, which is beneficial for visible light absorption [42]. When the visible light absorbed by C-STA@ZrO2 is higher than its own forbidden band width, the generation of the photogenerated electrons (e−) and holes (h+). e− jumps from the valence band (VB) of C-STA@ZrO2 to its conduction band (CB), while h+ stays on VB. The generated e− will be captured by O2 to form · O 2 − , and h+ will react with H2O to form ·OH. The dyes will react with the generated · O 2 − and ·OH, resulting in dyes that can be easily degraded in water.

Scheme 2 The possible photocatalytic reaction mechanism of C-STA@ZrO2 catalyst.
Scheme 2

The possible photocatalytic reaction mechanism of C-STA@ZrO2 catalyst.

4 Conclusion

In summary, the C-STA@ZrO2 composite was successfully prepared via the simple method. Through characterization, it was found that the good photocatalytic characteristic of photocatalytic degradation of organic pollutants in water for the C-STA@ZrO2 catalyst can be attributed to mesopore structure, high BET surface area and pore volume, and the interaction between STA and ZrO2, which improved the optical response. The degradation efficiency reached 93.9% in 120 min for RhB solution (40 mg·L−1) in the presence of C-STA@ZrO2 catalyst, and the catalyst can be recycled and reused. The synthesis method proposed in this study can be used to prepare MOF-derived metal oxide skeleton-based hybrids for environmental remediation.

  1. Funding information: This work was financially supported by the Project of Anshun University supporting Doctors Research ([2021]asxybsjj01), the Anshun Science and Technology Planning Project ([2021]1), the 2022 Innovative Entrepreneurship Training Program for Undergraduates of the Guizhou Education Department (202210667017), and the Student Research Training of Anshun University (asxysrt202202).

  2. Author contributions: Jialu Wang: writing – original draft, writing – review and editing, methodology, formal analysis, project administration; Rongfei Yu: methodology, formal analysis; Zhenying Li: methodology, formal analysis; Fen Yang: visualization; Linmin Luo: methodology, formal analysis; Dandan Wang: methodology, formal analysis; Huan Cheng: methodology, formal analysis; Yutao Zhang: visualization; Qiuyun Zhang: writing – review and editing, visualization.

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

  4. Data availability statement: The data implemented to support the results of the study are included within the manuscript.

Appendix

Figure A1 XRD patterns of obtained C-ZrO2, STA@UiO-66, and C-STA@ZrO2, and the reused C-STA@ZrO2 photocatalysts.
Figure A1

XRD patterns of obtained C-ZrO2, STA@UiO-66, and C-STA@ZrO2, and the reused C-STA@ZrO2 photocatalysts.

Figure A2 XRD patterns of the STA and UiO-66 samples.
Figure A2

XRD patterns of the STA and UiO-66 samples.

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Received: 2023-01-13
Revised: 2023-03-14
Accepted: 2023-03-28
Published Online: 2023-04-18

© 2023 the author(s), published by De Gruyter

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

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https://doi.org/10.1515/gps-2023-0005
Keywords for this article
metal–organic framework; silicotungstic acid; photocatalysis; rhodamine B; photodegradation
Creative Commons
BY 4.0

Articles in the same Issue

  1. Research Articles
  2. Value-added utilization of coal fly ash and recycled polyvinyl chloride in door or window sub-frame composites
  3. High removal efficiency of volatile phenol from coking wastewater using coal gasification slag via optimized adsorption and multi-grade batch process
  4. Evolution of surface morphology and properties of diamond films by hydrogen plasma etching
  5. Removal efficiency of dibenzofuran using CuZn-zeolitic imidazole frameworks as a catalyst and adsorbent
  6. Rapid and efficient microwave-assisted extraction of Caesalpinia sappan Linn. heartwood and subsequent synthesis of gold nanoparticles
  7. The catalytic characteristics of 2-methylnaphthalene acylation with AlCl3 immobilized on Hβ as Lewis acid catalyst
  8. Biodegradation of synthetic PVP biofilms using natural materials and nanoparticles
  9. Rutin-loaded selenium nanoparticles modulated the redox status, inflammatory, and apoptotic pathways associated with pentylenetetrazole-induced epilepsy in mice
  10. Optimization of apigenin nanoparticles prepared by planetary ball milling: In vitro and in vivo studies
  11. Synthesis and characterization of silver nanoparticles using Origanum onites leaves: Cytotoxic, apoptotic, and necrotic effects on Capan-1, L929, and Caco-2 cell lines
  12. Exergy analysis of a conceptual CO2 capture process with an amine-based DES
  13. Construction of fluorescence system of felodipine–tetracyanovinyl–2,2′-bipyridine complex
  14. Excellent photocatalytic degradation of rhodamine B over Bi2O3 supported on Zn-MOF nanocomposites under visible light
  15. Optimization-based control strategy for a large-scale polyhydroxyalkanoates production in a fed-batch bioreactor using a coupled PDE–ODE system
  16. Effectiveness of pH and amount of Artemia urumiana extract on physical, chemical, and biological attributes of UV-fabricated biogold nanoparticles
  17. Geranium leaf-mediated synthesis of silver nanoparticles and their transcriptomic effects on Candida albicans
  18. Synthesis, characterization, anticancer, anti-inflammatory activities, and docking studies of 3,5-disubstituted thiadiazine-2-thiones
  19. Synthesis and stability of phospholipid-encapsulated nano-selenium
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  21. Enrichment of low-grade phosphorites by the selective leaching method
  22. Electrochemical analysis of the dissolution of gold in a copper–ethylenediamine–thiosulfate system
  23. Characterisation of carbonate lake sediments as a potential filler for polymer composites
  24. Evaluation of nano-selenium biofortification characteristics of alfalfa (Medicago sativa L.)
  25. Quality of oil extracted by cold press from Nigella sativa seeds incorporated with rosemary extracts and pretreated by microwaves
  26. Heteropolyacid-loaded MOF-derived mesoporous zirconia catalyst for chemical degradation of rhodamine B
  27. Recovery of critical metals from carbonatite-type mineral wastes: Geochemical modeling investigation of (bio)hydrometallurgical leaching of REEs
  28. Photocatalytic properties of ZnFe-mixed oxides synthesized via a simple route for water remediation
  29. Attenuation of di(2-ethylhexyl)phthalate-induced hepatic and renal toxicity by naringin nanoparticles in a rat model
  30. Novel in situ synthesis of quaternary core–shell metallic sulfide nanocomposites for degradation of organic dyes and hydrogen production
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  48. Removal behavior of Zn and alkalis from blast furnace dust in pre-reduction sinter process
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  50. The mechanisms of inhibition and lubrication of clean fracturing flowback fluids in water-based drilling fluids
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  52. A one-pot, multicomponent tandem synthesis of fused polycyclic pyrrolo[3,2-c]quinolinone/pyrrolizino[2,3-c]quinolinone hybrid heterocycles via environmentally benign solid state melt reaction
  53. Green synthesis of silver nanoparticles using durian rind extract and optical characteristics of surface plasmon resonance-based optical sensor for the detection of hydrogen peroxide
  54. Electrochemical analysis of copper-EDTA-ammonia-gold thiosulfate dissolution system
  55. Characterization of bio-oil production by microwave pyrolysis from cashew nut shells and Cassia fistula pods
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  57. Photocatalytic research performance of zinc oxide/graphite phase carbon nitride catalyst and its application in environment
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  62. Silica-titania mesoporous silicas of MCM-41 type as effective catalysts and photocatalysts for selective oxidation of diphenyl sulfide by H2O2
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  65. Synthesis and characterization of Pluronic F-127-coated titanium dioxide nanoparticles synthesized from extracts of Atractylodes macrocephala leaf for antioxidant, antimicrobial, and anticancer properties
  66. Effect of pretreatment with alkali on the anaerobic digestion characteristics of kitchen waste and analysis of microbial diversity
  67. Ameliorated antimicrobial, antioxidant, and anticancer properties by Plectranthus vettiveroides root extract-mediated green synthesis of chitosan nanoparticles
  68. Microwave-accelerated pretreatment technique in green extraction of oil and bioactive compounds from camelina seeds: Effectiveness and characterization
  69. Studies on the extraction performance of phorate by aptamer-functionalized magnetic nanoparticles in plasma samples
  70. Investigation of structural properties and antibacterial activity of AgO nanoparticle extract from Solanum nigrum/Mentha leaf extracts by green synthesis method
  71. Green fabrication of chitosan from marine crustaceans and mushroom waste: Toward sustainable resource utilization
  72. Synthesis, characterization, and evaluation of nanoparticles of clodinofop propargyl and fenoxaprop-P-ethyl on weed control, growth, and yield of wheat (Triticum aestivum L.)
  73. The enhanced adsorption properties of phosphorus from aqueous solutions using lanthanum modified synthetic zeolites
  74. Separation of graphene oxides of different sizes by multi-layer dialysis and anti-friction and lubrication performance
  75. Visible-light-assisted base-catalyzed, one-pot synthesis of highly functionalized cinnolines
  76. The experimental study on the air oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid with Co–Mn–Br system
  77. Highly efficient removal of tetracycline and methyl violet 2B from aqueous solution using the bimetallic FeZn-ZIFs catalyst
  78. A thermo-tolerant cellulase enzyme produced by Bacillus amyloliquefaciens M7, an insight into synthesis, optimization, characterization, and bio-polishing activity
  79. Exploration of ketone derivatives of succinimide for their antidiabetic potential: In vitro and in vivo approaches
  80. Ultrasound-assisted green synthesis and in silico study of 6-(4-(butylamino)-6-(diethylamino)-1,3,5-triazin-2-yl)oxypyridazine derivatives
  81. A study of the anticancer potential of Pluronic F-127 encapsulated Fe2O3 nanoparticles derived from Berberis vulgaris extract
  82. Biogenic synthesis of silver nanoparticles using Consolida orientalis flowers: Identification, catalytic degradation, and biological effect
  83. Initial assessment of the presence of plastic waste in some coastal mangrove forests in Vietnam
  84. Adsorption synergy electrocatalytic degradation of phenol by active oxygen-containing species generated in Co-coal based cathode and graphite anode
  85. Antibacterial, antifungal, antioxidant, and cytotoxicity activities of the aqueous extract of Syzygium aromaticum-mediated synthesized novel silver nanoparticles
  86. Synthesis of a silica matrix with ZnO nanoparticles for the fabrication of a recyclable photodegradation system to eliminate methylene blue dye
  87. Natural polymer fillers instead of dye and pigments: Pumice and scoria in PDMS fluid and elastomer composites
  88. Study on the preparation of glycerylphosphorylcholine by transesterification under supported sodium methoxide
  89. Wireless network handheld terminal-based green ecological sustainable design evaluation system: Improved data communication and reduced packet loss rate
  90. The optimization of hydrogel strength from cassava starch using oxidized sucrose as a crosslinking agent
  91. Green synthesis of silver nanoparticles using Saccharum officinarum leaf extract for antiviral paint
  92. Study on the reliability of nano-silver-coated tin solder joints for flip chips
  93. Environmentally sustainable analytical quality by design aided RP-HPLC method for the estimation of brilliant blue in commercial food samples employing a green-ultrasound-assisted extraction technique
  94. Anticancer and antimicrobial potential of zinc/sodium alginate/polyethylene glycol/d-pinitol nanocomposites against osteosarcoma MG-63 cells
  95. Nanoporous carbon@CoFe2O4 nanocomposite as a green absorbent for the adsorptive removal of Hg(ii) from aqueous solutions
  96. Characterization of silver sulfide nanoparticles from actinobacterial strain (M10A62) and its toxicity against lepidopteran and dipterans insect species
  97. Phyto-fabrication and characterization of silver nanoparticles using Withania somnifera: Investigating antioxidant potential
  98. Effect of e-waste nanofillers on the mechanical, thermal, and wear properties of epoxy-blend sisal woven fiber-reinforced composites
  99. Magnesium nanohydroxide (2D brucite) as a host matrix for thymol and carvacrol: Synthesis, characterization, and inhibition of foodborne pathogens
  100. Synergistic inhibitive effect of a hybrid zinc oxide-benzalkonium chloride composite on the corrosion of carbon steel in a sulfuric acidic solution
  101. Review Articles
  102. Role and the importance of green approach in biosynthesis of nanopropolis and effectiveness of propolis in the treatment of COVID-19 pandemic
  103. Gum tragacanth-mediated synthesis of metal nanoparticles, characterization, and their applications as a bactericide, catalyst, antioxidant, and peroxidase mimic
  104. Green-processed nano-biocomposite (ZnO–TiO2): Potential candidates for biomedical applications
  105. Reaction mechanisms in microwave-assisted lignin depolymerisation in hydrogen-donating solvents
  106. Recent progress on non-noble metal catalysts for the deoxydehydration of biomass-derived oxygenates
  107. Rapid Communication
  108. Phosphorus removal by iron–carbon microelectrolysis: A new way to achieve phosphorus recovery
  109. Special Issue: Biomolecules-derived synthesis of nanomaterials for environmental and biological applications (Guest Editors: Arpita Roy and Fernanda Maria Policarpo Tonelli)
  110. Biomolecules-derived synthesis of nanomaterials for environmental and biological applications
  111. Nano-encapsulated tanshinone IIA in PLGA-PEG-COOH inhibits apoptosis and inflammation in cerebral ischemia/reperfusion injury
  112. Green fabrication of silver nanoparticles using Melia azedarach ripened fruit extract, their characterization, and biological properties
  113. Green-synthesized nanoparticles and their therapeutic applications: A review
  114. Antioxidant, antibacterial, and cytotoxicity potential of synthesized silver nanoparticles from the Cassia alata leaf aqueous extract
  115. Green synthesis of silver nanoparticles using Callisia fragrans leaf extract and its anticancer activity against MCF-7, HepG2, KB, LU-1, and MKN-7 cell lines
  116. Algae-based green AgNPs, AuNPs, and FeNPs as potential nanoremediators
  117. Green synthesis of Kickxia elatine-induced silver nanoparticles and their role as anti-acetylcholinesterase in the treatment of Alzheimer’s disease
  118. Phytocrystallization of silver nanoparticles using Cassia alata flower extract for effective control of fungal skin pathogens
  119. Antibacterial wound dressing with hydrogel from chitosan and polyvinyl alcohol from the red cabbage extract loaded with silver nanoparticles
  120. Leveraging of mycogenic copper oxide nanostructures for disease management of Alternaria blight of Brassica juncea
  121. Nanoscale molecular reactions in microbiological medicines in modern medical applications
  122. Synthesis and characterization of ZnO/β-cyclodextrin/nicotinic acid nanocomposite and its biological and environmental application
  123. Green synthesis of silver nanoparticles via Taxus wallichiana Zucc. plant-derived Taxol: Novel utilization as anticancer, antioxidation, anti-inflammation, and antiurolithic potential
  124. Recyclability and catalytic characteristics of copper oxide nanoparticles derived from bougainvillea plant flower extract for biomedical application
  125. Phytofabrication, characterization, and evaluation of novel bioinspired selenium–iron (Se–Fe) nanocomposites using Allium sativum extract for bio-potential applications
  126. Erratum
  127. Erratum to “Synthesis, characterization, and evaluation of nanoparticles of clodinofop propargyl and fenoxaprop-P-ethyl on weed control, growth, and yield of wheat (Triticum aestivum L.)”
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