APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Wei Li,Xiao Wang,Min Li,Shu-ao He,Qiong Ma,Xuechuan Wang
Hydrogen is known as an alternative new energy for its advantages of non-pollution and high calorific value, and photocatalysis technology is regarded as one of the most effective means to produce hydrogen in recent years. In this topic, aiming at the poor photoresponse, fast combination of photo-induced carriers and unstable structure of traditional photocatalysts, the three-dimensional porous g-C 3 N 4 /graphene oxide framework was constructed by compounding two-dimensional graphene oxide and two-dimensional g-C 3 N 4 via hard template (SiO 2 nanoparticles) method and selective chemical etching. Then, silver bromide nanoparticles , a superior photosensitizer, were immobilized on the three-dimensional porous framework to construct the three-dimensional porous g-C 3 N 4 /graphene oxide-AgBr photocatalyst with Ag plasmas by solvothermal method. Research showed that this novel photocatalyst based on Z-scheme heterostructure (GO-AgBr), p-n heterostructure (g-C 3 N 4 -AgBr) and Ag plasmas presented high-efficient visible-light driven hydrogen evolution (3.69 mmol/g/h) at the absence of Pt co-catalyst, which is higher than the majority of existing catalysts, and it also possessed strong stability on its activity and structure. Accordingly, the enhanced hydrogen evolution and photostability were attributed to the highly ordered structure and fast interfacial electron conduction of three-dimensional porous framework, superior photosensitivity of AgBr and synergistic effect of Ag plasmas. Therefore, this study provided a potential method for exploitation of hydrogen energy.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Chaoting Guan,Jin Jiang,Suyan Pang,Xiao Chen,Richard D. Webster,Teik-Thye Lim
Previous studies have reported that metal-doped graphitic carbon nitride (g-C 3 N 4 ) materials can activate peroxymonosulfate (PMS) to destruct organic pollutants. Herein, we interestingly found that pure g-C 3 N 4 materials synthesized via a facile calcination protocol without any metal doping could serve as the efficient PMS activator for degrading bisphenol A (BPA). The influences of different precursors (i.e., melamine, dicyandiamide, and urea) and annealing ambience (i.e., air or N 2 ) on the catalytic activity were investigated. The resultant g-C 3 N 4 materials exhibited different catalytic activities for PMS activation. The best performance was found in the case of g-C 3 N 4 synthesized from melamine and annealed in N 2 (g-C 3 N 4 -Melamine-N 2 ); 100% BPA (10 μM) removal was achieved by using 0.5 g/L catalyst and 1 mM PMS at pH 7 in 15 min. The difference in catalytic activities of these g-C 3 N 4 materials might be attributed to the fact that different preparation procedures impacted the chemical composition and structure of catalysts and thus changed the type and density of active sites. Important influencing factors such as PMS dosage, temperature, solution pH, and water matrices on degradation kinetics of BPA were evaluated. Results of quenching experiments and electron paramagnetic resonance spectroscopy revealed that sulfate radical and hydroxyl radical were main reactive species for BPA degradation by the g-C 3 N 4 /PMS system, which was also confirmed by the non-selectivity of this system towards various organics. Furthermore, possible transformation pathways of BPA by the g-C 3 N 4 /PMS system were proposed based on the identified oxidation products, primarily involving hydroxylation, bond cleavage, ring opening, as well as radical coupling. This study deepens mechanistic understanding of g-C 3 N 4 materials driven PMS oxidation processes, and also provides a green and efficient strategy for eliminating BPA in water.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Wenxia Wang,Zhen Li,Han Wang,Hangyu Luo,Zhenbang Meng,Xiaofeng Liu,Lingyu Liu,Weirui Chen,Baosheng Jin,Kai Huang,Ri Chen,Qi He
Dual Z-scheme heterojunction with highly separation efficiency of photoinduced carriers and outstanding redox capability has received considerable attention and hold great promise for environmental remediation. Herein, magnetic dual Z-scheme g-C 3 N 4 /ZnFe 2 O 4 /Ag 2 CO 3 heterojunction was successfully constructed, and applied as a dual-function photocatalyst for tetracycline (TC) degradation and bacterial inactivation. The optimized g-C 3 N 4 /ZnFe 2 O 4 /Ag 2 CO 3 heterojunction exhibited excellent photocatalytic capacity for TC degradation with a rate constant of 0.0154 min −1 , which is 2.73, 3.08, and 2.92 times higher compared to that of the g-C 3 N 4 , ZnFe 2 O 4 , and g-C 3 N 4 /ZnFe 2 O 4 , respectively. Impressively, the g-C 3 N 4 /ZnFe 2 O 4 /Ag 2 CO 3 -1.25 heterojunction displayed satisfying activity within a wider range of pH (3.0–9.0), TC concentration (5–25 mg L −1 ), and with the addition of various anions including Cl - , HCO 3 - , SO 4 2- , and NO 3 - . Meanwhile, 6.5-log of Escherichia coli cells could also be inactivated by g-C 3 N 4 /ZnFe 2 O 4 /Ag 2 CO 3 -1.25 heterojunction under visible light. Mechanism exploration based on trapping experiment, electron paramagnetic resonance (EPR) analysis, and liquid chromatography-mass spectrometer (LC-MS) indicated that the improved photocatalytic performance resulted from the synergetic effect of semiconductors and constructed dual Z-scheme heterojunction, which significantly promotes charge separation rate and endows strong redox capacity. As expected, the toxicity of TC degradation intermediates was reduced according to the Toxicity estimation analysis based on a quantitative structure activity relationships (QSAR) method. Further, the g-C 3 N 4 /ZnFe 2 O 4 /Ag 2 CO 3 heterojunction also demonstrated magnetic separation property and satisfactory photocatalytic stability even after 4 cycles. This work offers a new perspective on constructing novel magnetic dual Z-scheme heterojunction with dual-function photocatalytic properties and is of significance for water remediation.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Xian Li,Weilong Zhang,Xiaojun Wen,Lijun You,Jumei Li
Magnetically separable Fe 3 O 4 /hTiO 2 /g-C 3 N 4 composites were successfully constructed through coating polymethylacrylic acid sacrificial interlayer by the reflux-precipitation polymerization and subsequent TiO 2 outer layer by sol–gel method over magnetic Fe 3 O 4 nanospheres, calcining process and forming composites with g-C 3 N 4 in sequence . The formation mechanism of unique composites was proved by TEM, XPS, VSM, XRD and EDX mapping characterization. Their photocatalytic activity was investigated by the solar photodegradation of organic dyes. The results revealed the photocatalytic performance of Fe 3 O 4 /hTiO 2 /g-C 3 N 4 for degrading methylene blue (95.0 %, 120 min) under simulated sunlight irradiation (Xe lamp, 500 W) was much better than g-C 3 N 4 (71.1 %, 120 min) and Fe 3 O 4 /hTiO 2 (40.3 %, 120 min). The boosted property is presumably ascribed to the synergetic interaction of multiple components and effective separation of the photoproduced electron-hole pairs between g-C 3 N 4 and TiO 2 , which was verified using photocurrent and EIS analysis. On the basis of the scavenging studies of radicals ( h + , •O 2 – and •OH), the mechanism of the boosted photocatalytic performance was put forward. The degradation pathways of methylene blue were also proposed by identifying reaction intermediates produced during photocatalysis. More significantly, the composites presented excellent magnetic responsive property owing to the magnetic Fe 3 O 4 . The superior recyclability was confirmed by cyclical photocatalytic experiments with the help of an external magnet, which is crucial for the sustainable and green application of photocatalysts.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Guorui Chang,Sirui Li,Yunqi Wang,Qingxia Ran,Qing Tan,Shuli Gou,Haiying Du,Shuxia Xu
Rapid detection of pesticide residues in vegetables has recently attracted much attention. Herein, a Cu-modified graphitic carbon nitride nanomaterial (Cu-C 3 N 4 ) with peroxidase (POD)-like property was synthesized to construct an enzyme-based colorimetric sensing platform for the detection of organophosphorus pesticides paraoxon . Cu-C 3 N 4 could catalyze H 2 O 2 produced by reaction of acetylcholine with acetylcholinesterase and choline oxidase, and then further oxidized 3,3,5,5-tetramethylbenzidine (TMB) to produce a blue colored product. Presence of organophosphorus pesticide paraoxon (PA) restrained the activity of acetylcholinesterase AChE, triggering a remarkably decreased amount of H 2 O 2 towards TMB oxidation, which led to the inhibition of oxidation reaction. After that, the reaction solutions were freeze-dried in a portable bioactive capsule with addition of trehalose as stabilizer for improved enzymes activities . On the basis of the variation in gray-scale values of blue colored TMB solutions using an application, a smartphone-based 3D printing platform was obtained with a linear range from 100 to 33,000 nM (R 2 = 0.994) and a detection limit of 13 nM (3 σ/k ). This smartphone-based 3D-printed colorimetric platform combined with a bioactive capsule offers a novel approach with the potential for rapid detection of PA in vegetables.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Qi-Xin Wei,Ai-Yong Zhang,Zedong Yang,Song Hu,De-Jin Wang,Chi Zhang,Chang Liu,Rui Liu
Solid catalyst plays the governing role in the heterogeneous Fenton-like catalysis for water purification . In this work, the Co(II)-doped C 3 N 4 (Co/C 3 N 4 ) was prepared and further thermally exfoliated in different atmosphere for the three-dimensional layered configuration. The morphological and structural properties as well as surface chemistry of Co/C 3 N 4 before and after thermal exfoliation were elucidated in comparison. The oxygen-exfoliated Co/C 3 N 4 (O-Co/C 3 N 4 ) exhibited accessible metal exposure and synergistic pollutant adsorption stemmed from three-dimensional layered configuration with ordered porous configuration, oriented lamellar structure and increased surface area. Moreover, an excellent Fenton-like reactivity and stability was measured for PMS activation and pollutant degradation , and the comparative performance before and after oxygen exfoliation as well as with typical metal-based catalysts were investigated in details. The impacts of testing conditions and water matrices were elucidated to estimate environmental potential. Based on radical identifying and inhibiting tests and electrochemical measurements, the non-radical reaction pathway from mediated electron transfer (MET) played the key role with much reduced matrix effects and satisfactory catalytic selectivity . This work provides a new chance to save transition-metal consumption and refine Fenton-like reactivity in C 3 N 4 -based catalysts for superior environmental remediation.
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高影响因子
CORROSION SCIENCE
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2023
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IF 8.3
Yiqian Lv,Wenjie Zhao,Yujie Qiang,Jingmao Zhao
Based on high barrier performance, the combination of active/passive self-repairing and early corrosion monitoring functions becomes an ideal anti-corrosion strategy. Abundant surface polar functional groups of carbon quantum dots (CQDs) made of juice helped graphite carbon nitride(g-C 3 N 4 ) compatible with epoxy resin, and effectively improved the barrier property of CQDs@g-C 3 N 4 composites in coatings. In addition, the adsorption of CQDs on metal is the source of the active protective performance of the coating. The fluorescence characteristics of CQDs made it realizable to detect the micro-cracks in coatings. This work provides a meaningful strategy for the design of intelligent protective materials.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yuhang Zhou,Jiafeng Ding,Wen Yan,Yunjuan Meng,Bingzhi Yu,Teer Wen,Yao Yue,Yuchi Zhong,Hangjun Zhang
Degradation of endocrine disrupting compounds by optimizing advanced oxidation processes is highly feasible, but remains a daunting challenge. In this work, a novel copper and molybdenum co-doped g -C 3 N 4 (Cu/Mo@CN) were successfully synthesized via a simple dip-calcination approach, of which highly dispersed Cu and Mo atom sites were doped in the ring of g -C 3 N 4 . The Cu/Mo@CN catalysts were characterized by XRD, SEM, TEM, XPS, UV–vis DRS analyses, etc. The optimized system of Cu 1 /Mo 3 @CN catalyst in the visible light-persulfate oxidation (Vis + PS + Cu 1 /Mo 3 @CN system) had high photocatalytic activity to remove 97.2 % of bisphenol A (BPA, 5 mg/L) within 60 min. Compared to pure g -C 3 N 4 , Cu/Mo@CN has better visible-light (Vis) response function and narrower band gap (2.58 eV), which are easier to get excited by Vis illuminate. The results showed that reactive oxygen species of SO 4 • − , • OH and • O 2 − could be stably produced to contribute to the BPA degradation in Vis + PS + Cu/Mo@CN systems. Meanwhile, the Cu and Mo elements co-doped in g -C 3 N 4 can also effectively activate PS to promote the production of reactive oxygen substances. In addition, the continuous production of photoelectrons enhanced the cycling of Cu 2+ /Mo 6+ and Cu + /Mo 4+ , which could be further improved the removal efficiency of Vis + PS + Cu/Mo@CN towards BPA. The degradation mechanism of BPA were proposed according to the identification of intermediate products and DFT calculation. Overall, this study provides a viable pathway for BPA abatement in actual wastewater treatment applications.
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Xin Yan,Na Zhang,Zhiliang Liu,Chunfang Du
In this paper, 1T/2H mixed-phase MoS 2 /g-C 3 N 4 composites (1T/2H-MG) were successfully synthesized by a simple two-step calcination method and used for Cr(VI) removal from aqueous environment. A series of characterization methods were used to characterize the microstructure and surface morphology of the prepared materials. The experiment results showed that 1T/2H-MG (1:12) composite with good pH and temperature adaptability could completely remove Cr(VI) (100 mg∙L –1 ) within 50 min and showed an excellent adsorption capacity of 342.06 mg∙g –1 . The presence of abundant sulfur defects in 1T/2H-MG composite could provide more adsorption and reduction active sites, which was the main reason for the enhanced removal efficiency of 1T/2H-MG in comparison with pure MoS 2 and g-C 3 N 4 . This work not only contributes an excellent adsorbent for the wastewater treatment, but also provides evidences for the defects engineering.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Qian Li,Jiahui Zhang,Jiayu Zhou,Wang Xu,Zhuowei Cheng,Piet N.L. Lens,Jianmeng Chen,Dongzhi Chen
The effective and economic treatment of chlorobenzenes has become one of the most intractable issues in the field of air pollution control. Herein, a visible-light photocatalysis coupled with biodegradation (VPCB) system was developed by integrating an innovative visible-light responsive TiO 2 /oxygenous groups decorated g-C 3 N 4 (TiO 2 /OCN) with polyurethane carriers immobilized with Ralstonia sp. XZW-1 for chlorobenzene removal. Performance tests showed that light intensity, preparation of the MICs, catalyst dosage and composition of the TiO 2 /OCN cast significant influence on chlorobenzene removal efficiency, with the degradation efficiency, mineralization and dechlorination ratios of VPCB achieving 100%, 35.5%, and 99.4% under the optimal conditions, respectively, outcompeting the sum of visible-light photocatalytic system and biodegradation protocols. Cycling tests further demonstrated the excellent stability of VPCB. Mechanism analysis found that increased reactive sites, improved visible-light harvesting, accelerated charge transfer and separation, and the resulting abundant active species jointly contributed to the enhanced photocatalytic activity of TiO 2 /OCN. Photogenerated holes were most significant active species for chlorobenzene removal, followed by OH and O 2 − radicals. The carriers could effectively protect microorganisms from light illumination and strong oxidizing species, allowing the further microbial metabolism of chlorobenzene photocatalytic oxidation intermediates with good biodegradability, not only greatly promoting the microbial growth and activity, but further enhancing chlorobenzene photocatalytic degradation. Plausible synergistic mechanism for chlorobenzene degradation between photocatalysis and biodegradation was also revealed. Furthermore, the VPCB system constructed presented wide applicability towards various pollutants, and its performance was found closely related with the hydrophobicity of pollutants. This work provided insight into the design and application of the VPCB system for the efficient and economic treatment of refractory pollutants.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Qian Zhai,Jingde Luan,Xin Ke,Wengang Liu,Zheng Yan
Flash photodegradation of organic pollutants at high concentrations is an urgent need for industrial organic wastewater treatment. Situ high-energy wet ball milling is adopted to fabricate the vanadium-oxygen doped carbon nitride catalysts to implement the flash degradation of methylene blue (MB). The experimental results indicated that the photocatalyst degradation ratio of MB was higher than 90% in 3 min under visible-light irradiation 300 W, catalyst dosage 0.2 g/L and MB concentration of 100 mg/L. MB removal rate was nearly 20 times higher than that of primitive carbon nitride. Vanadium-oxygen doping was beneficial to the reduction of band gap less than 2.0 eV and the formation of built-in electric field. It is notable notice that both valence band and conduction band of catalyst were tuned to be in positive potential region, benefiting for holes (h + ) formation to boost the flash degradation of contaminants. Strong electrophilic attack of h + caused the bonds of C-S + =C and C N-C broken, triggering the aromatic ring opened to decompose into smaller molecules.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Xinyu Li,Fei Ye,Hui Zhang,Munir Ahmad,Zhenxing Zeng,Shuaijie Wang,Sufeng Wang,Dawei Gao,Qingrui Zhang
Integrating g-C 3 N 4 with narrow-band semiconductor to construct a Z-scheme structured heterojunction has been regarded as a common strategy to improve the photocatalytic performance of g-C 3 N 4 . However, limited catalytic activity increment is achieved due to the contradiction of expanding the light absorption scope of traditional photo-oxidation semiconductors (PS II) and preserving their valance band oxidative abilities. Herein, to extend the light absorption range of g-C 3 N 4 based Z-scheme photocatalyst to the whole solar spectra while without losing the high oxidative ability of this system, we select the heavy doped W 18 O 49 as PS II and provide a facile in situ hydrothermal method to elaborately fabricate an rGO decorated W 18 O 49 @g-C 3 N 4 (r-CNW) Z-scheme photocatalyst. The prepared r-CNW-2 (with optimal W 18 O 49 to g-C 3 N 4 weight ratio of 1:2) exhibits improved photocatalytic performance with H 2 O 2 generation rates of 71, 58.5 and 6.3 μmol g −1 h −1 obtained under the simulated solar light, visible light (>400 nm) and NIR light (>800 nm) irradiation, respectively, which is 1.3 and 2 times higher than those of the g-C 3 N 4 counterparts (54, 29 μmol g −1 h −1 and even not detected).such outstanding performance of r-CNW-2 could be associated with the broader light absorption, fast charge separation, and rapid redox reactions. Moreover, the r-CNW-2 also displays an excellent E-coli inactivation activity, comparable to most g-C 3 N 4 -based photocatalysts. Our work gives a new insight through trading off light absorption and redox ability to fabricate efficient Z-scheme photocatalyst for photocatalytic H 2 O 2 generation and environmental remediation.
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危险品化学品经营许可证（带存储）