CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Zhijie Zhang,Xuesheng Wang,Huiling Tang,Deben Li,Jiayue Xu
Modulating the internal electric field (IEF) represents a potential strategy to stimulate the photocatalytic activity of heterojunctions, especially S-scheme photocatalysts. Herein, a Cs 3 Bi 2 Br 9 @V O -In 2 O 3 (CBB@V O -In 2 O 3 ) S-scheme heterojunction, of which Cs 3 Bi 2 Br 9 perovskite quantum dots (PQDs) are embedded into mesoporous V O -In 2 O 3 hosts, is rationally designed as a cornerstone for further IEF manipulation. Briefly, by introducing oxygen vacancies (V O ) into the composed reduction semiconductor (mesoporous In 2 O 3 ), an enlarged Fermi level ( E F ) gap between CBB and V O -In 2 O 3 is achieved, yielding an intensified IEF over the CBB@V O -In 2 O 3 heterojunction. Such an enhanced IEF affords a much more robust driving force for directional carrier delivery, leading to accelerated carrier transfer of CBB@V O -In 2 O 3 heterojunction. Consequently, the optimized CBB@V O -In 2 O 3 heterojunction features desirable CO 2 -to-CO conversion efficiency, and its CO production rate reaches 130.96 μmol g −1 h −1 . The reaction intermediates and CO 2 photoconversion pathway were unraveled by in-situ diffuse reflectance infrared Fourier transform spectroscopy. Combining with the DFT calculation, it was revealed that oxygen vacancies in V O -In 2 O 3 act as reactive centers, which optimize the coordination modes of the intermediates, thus reducing the activation energy for photocatalytic CO 2 reduction. Our work demonstrates that the IEF modulation of S-scheme-based heterojunction could significantly boost the charge separation and then to drive efficient catalytic reaction , achieving high-efficiency solar fuel production.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ting Liang,Zebin Yu,Yuejing Bin,Shiming Zhang,Jingwen Wei,Yujia Liu,Tingting Zhu,Songyu Fan,Yuxiang Shen,Shuangfei Wang,Yanping Hou
Inefficient separation and sluggish transfer of photogenerated charges on the photocatalyst is one of the bottlenecks for CO 2 photocatalytic reduction. In this study, the ZnSe/ZnWO 4 heterojunction with tungsten vacancies and oxygen vacancies (ZZ-30%-Vw,o) was synthesized by hydrothermal process and post-etching method for CO 2 reduction. Various characterizations showed superior structural and optical properties of the ZZ-30%-Vw,o heterojunction; results of ESR and work function calculation demonstrated that the heterojunction conformed to S-scheme charge transfer mechanism. Results of various tests and density functional theory (DFT) calculation confirmed the existence of W and O vacancies, as well as the locally polarized electric field (PEF). The PEF and the built-in electric field (IEF) could not only accelerate carriers separation and transfer, but also enhance CO 2 adsorption and activation, thus enhancing photocatalytic activity toward CO 2 reduction. The ZZ-30%-Vw,o composite exhibited the highest CO yield of 96.91 µmol/g/h, approximately 21.0 times of the ZnSe . Moreover, the ZZ-30%-Vw,o possessed favorable structure-performance stability. The COOH* was the most important intermediate during CO 2 reduction, and possible CO 2 reduction pathways and mechanism were proposed. This work paves a feasible way for improving photocatalytic activity via introducing dual surface vacancies on heterojunction photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kaiyuan Shen,Yu Tang,Qihang Zhou,Ying Zhang,Wen Ge,Xuxia Shai,Shuping Deng,Peizhi Yang,Shukang Deng,Jinsong Wang
Development of economical and high-efficient catalytic electrodes is a top priority for oxygen evolution reactions (OER). Non-precious metal based metal–organic frameworks (MOFs) in powder form remain a series of problems including the assistance of adhesive, poor conductivity and stability. Herein, a well-designed S-NiFe PBA@NiFe/NF composite with a unique Mott-Schottky heterojunction architecture was purposefully constructed by self-sacrificing template approach and electrodeposition. The growth of S-NiFe PBA@NiFe on NF through in situ synthesis promotes efficient electron conduction between the NF substrate and S-NiFe PBA@NiFe catalyst, leading to a stable and highly effective working state. The Mott-Schottky heterojunctions between S-NiFe PBA and NiFe-layered double hydroxides (LDH) effectively expedite electronic transmission. Consequently, S-NiFe PBA@NiFe/NF exhibits outstanding OER behavior at 1.0 M KOH, exhibiting a low Tafel slope of 39 mV dec −1 and at 10 mA cm −2 , reaching an unexpectedly low overpotential of 196.7 mV. Furthermore, the S-NiFe PBA@NiFe/NF maintains long-term durability without evident performance degradation for 100 h.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Zhentao Bian,Meng Li,Taoqin Liu,Chengcheng Liu,Yanyan Zhu,Hongxia Cao,Guang Zhu,Hongyan Wang,Chong Chen,Keying Zhang
Recent research interest has increased in the production of heteroatoms-doped porous carbon with controlled morphology from biomass. However, there is still a significant challenge in resolving alkaline solutions that cause equipment corrosion and devising a simple and adaptable approach. In this study, N/O/S co-doped honeycomb-like porous carbons were synthesized from a widely cultivated annual weed ( Hemistepta Iyrata Bunge ) using a simple and eco-friendly method. The sodium hydroxide (NaOH)/urea system was utilized as the pore-forming agent and cellulose solvent, with urea as the nitrogen source. By varying the activation temperature, the as-prepared porous carbon has a high specific surface area (709 m 2 g −1 ), a large total pore volume (0.44 cm 3 g −1 ), and a high heteroatom content of 6.20 at% nitrogen and 8.12 at% oxygen. The prepared porous materials were evaluated as electrodes for supercapacitors . The product (HIB-PHC-750 °C) exhibited a high specific capacitance (353.6 F g −1 at 0.2 A g −1 ) at a carbonization temperature of 750 °C. Additionally, the HIB-PHC-750 °C-based symmetric device with a wide voltage range of 2.0 V possessed a desirable energy density of 44.22 Wh kg −1 at 500 W kg −1 . Moreover, the HIB-PHC-750 °C also demonstrated outstanding cycling stability with 98.2 % capacitance retention after 10,000 cycles. This research provided a facile and favorable alternative method for preparing N/O/S co-doped honeycomb-like porous carbon for electrochemical energy storage devices.
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ENVIRONMENTAL POLLUTION
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2023
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IF 8.9
Yang Wang,Shuang Yu,Hongwei Yuan,Lei Zhang
To solve the problem of biochar lack of adsorption sites for heavy metal ions and the difficulty of recycling, CoFe 2 O 4 magnetic nanoparticles confined in nitrogen, sulfur co-doped 3D network biochar matrix (C–CoFe 2 O 4 /N,S-BC) was designed and fabricated successfully. The obtained C–CoFe 2 O 4 /N,S-BC displays remarkable adsorption performance for both Pb 2+ and ciprofloxacin (CIP) removal at the single or binary system due to the role of N,S as metal ion anchoring compared to the N,S-free sample (CoFe 2 O 4 /BC). N,S co-doped BC not only participates in adsorption reaction but also effectively inhibites the agglomeration of CoFe 2 O 4 nanoparticles and increases the active sites as a carrier at the same time. In the single system, CoFe 2 O 4 /N,S-BC demonstrates a fast adsorption rate (equilibrium time: 30 min) and high adsorption capacity (224.77 mg g −1 for Pb 2+ , 400.11 mg g −1 for CIP) towards Pb 2+ and CIP. The adsorption process is befitted pseudo-second-order model, and the equilibrium data are in great pertinence with Langmuir model. In the binary system, the maximum adsorption capacity of CoFe 2 O 4 /N,S-BC for Pb 2+ and CIP is 244.80 mg g −1 (CIP: 10.00 mg L −1 ) and 418.42 mg g −1 (Pb 2+ : 10.00 mg L −1 ), respectively. The adsorption mechanism is discussed based on the experimental results. Moreover, C–CoFe 2 O 4 /N,S-BC shows good practical water treatment capacity, anti-interference ability and stable reusability (the removal efficiency＞80% after eight cycles). The rapid, multifunctional, reusable, and easily separable adsorption properties make C–CoFe 2 O 4 /N,S-BC promising for efficient environmental remediation. This study also offers a viable method for the construction of adsorption material for complex wastewater treatment .
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Guanwei Peng,Yanyu Xie,Ying Wang,Qi Yu,Youyi Huang,Shuwu Liu,Limin Lu
Peroxymonosulfate (PMS)-assisted photocatalytic processes are economical and green strategies for the treatment of pesticide pollution. However, its degradation efficiency is severely hindered by the sluggish kinetics of active centers regeneration and low charge-transfer. Herein, S-scheme Bi 2 Fe 4 O 9 /BiOBr heterogeneous material was designed to activate PMS for thiabendazole (TBZ) degradation. Bi 2 Fe 4 O 9 and BiOBr have similar structural unit of [Bi 2 O 2 ] 2+ to share the Bi-O bonds, which is favorable to form asymmetric interface and enhance the polarization. Based on these unique characteristics between Bi 2 Fe 4 O 9 and BiOBr, a robust internal electric field in the S-scheme heterojunction is built, which could provide driving force to boost the electron-transfer process and encourage the sustainable regeneration of Fe 2+ . After optimizing the proportion of Bi 2 Fe 4 O 9 on the composite, it was found that 50 wt% Bi 2 Fe 4 O 9 /BiOBr (BFB-50) exhibits the best TBZ removal efficiency after 30 min visible light irradiation, which is 2.25 and 12 folds compared to Bi 2 Fe 4 O 9 and BiOBr, respectively. Furthermore, electron paramagnetic resonance (EPR) and radical trapping experiments indicate that 1 O 2 and SO 4 •- involving oxidation mechanism impart maximum contribution towards TBZ degradation. The possible pathways of TBZ degradation are reasonably proposed by the HPLC-MS and the toxicity evolution of TBZ is appraised using the ECOSAR software. This study provides an insight into the fabrication of S-scheme heterojunction for environment remediation through the photocatalysis/sulfate-mediated advanced oxidation process.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Yuwei Ding,Meng Li,Qian Zhang,Yibo Zhang,Zhixuan Xia,Xiangyu Liu,Nanping Wu,Jie Peng
To improve the performance of the nanoscale zero-valent iron (nZVI)-based advanced oxidation process (AOPs), a sulfidation pre-modification endowed nZVI with stable reduction nature mechanism was proposed, and a coupled system of activating PMS with sulfidized nanoscale zero-valent iron supported by biochar(S-nZVI/BC@PMS) was constructed in this study. It could be found that sulfidation state and formation, largely dependent on the sulfidized modification method, had a great impact on the enhancement for nZVI/BC in activating PMS for Acid Red 73 degradation. Compared with original nZVI/BC, the formed FeS shell blocked the external air to protect the internal Fe 0 , and S-nZVI/BC became relatively hydrophobic, which could slow down the material corrosion by water and dissolved oxygen to enhance the reaction durability. Appropriate sulfidation reduced the electrochemical impedance and enhanced the electrical conductivity of the catalyst, which facilitated the electron transfer in the system, and the participation of reducing sulfur species enabled the reaction to form a positive cycle and ensure a prolonged duration. Excessive sulfidation caused the material to become unstable and thus susceptible to air erosion, reducing the efficiency of contaminant removal. Due to the FeS protective shell, hydrophobicity of S-nZVI/BC and the promoted electron transfer in the system, S-nZVI/BC@PMS system secured more free radicals and had longer reaction time under the same conditions. In addition, S-nZVI/BC had good antioxidant properties, universality, and reusability for practical applications. These findings not only elucidated the superiority of S-nZVI/BC@PMS system but also provided new insights into cost-saving and efficient advanced oxidation processes.
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OPTICAL MATERIALS
·
2023
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IF 3.9
Vu Hoang Huong,Van-Can Nguyen,Minh Ngoc Ha,Duy Van Pham,Thanh Binh Nguyen,Yuan-Ron Ma,An Bang Ngac,Trinh Thi Loan
The photo-Fenton process serves as a highly efficient approach for removing contaminants from wastewater. In this study, we developed a Fe-doped TiO 2 /SnO 2 heterojunction catalyst to enhance the efficiency of photo-Fenton catalytic activity under visible light . To investigate the physical properties of the catalysts, various characterization techniques were utilized, including XRD , SEM, TEM , HR-TEM, UV-VIS, PL , and XPS . The 7% mol Fe-doped TiO 2 /SnO 2 -OVs (TFS-7) heterostructure exhibited the highest rate constant of 17.03 × 10 −3 min −1 ; 8.4 and 2.1 times higher than the individual components. This enhanced performance is mainly attributed to the rapid migration of photoinduced electrons to Fe 3+ and the subsequent generation of Fe 2+ , which improved electron transfer capacity and facilitated the rapid production of hydroxyl radicals (•OH) through the reaction between Fe 2+ and H 2 O 2 . We proposed a S-scheme mechanism for the Fe-doped TiO 2 /SnO 2 -OVs catalyst based on the analysis of reactive species trapping experiments, photoluminescence (PL) spectra, ultraviolet photoelectron spectroscopy (UPS), and density functional theory (DFT). These findings offer not only a straightforward approach for synthesizing highly active photocatalysts for the degradation of RhB dye, but also a framework for the construction of heterostructure photocatalysts.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 19
·54556-54567
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IF 5.8
Zhang Ge,Yang Huifen,Li Xuan,Zhou Yichen,Guo Song,Zhao Tong
The control of multiple heavy metals (HMs) pollution in solid wastes, especially the co-contamination of As and other heavy metal cations, is of great importance to ecological and environmental health. To address this problem, the preparation and application of multifunctional materials have attracted wide attention. In this work, a novel Ca-Fe-Si-S composite (CFSS) was applied to stabilize As, Zn, Cu, and Cd in acid arsenic slag (ASS). The CFSS exhibited synchronous stabilization ability for As, Zn, Cu, Cd and owned strong acid neutralization capacity. Under simulated field conditions, the acid rain extracted HMs in ASS successfully decreased below the emission standard (GB 3838–2002-IV category in China) after incubated by 5% CFSS for 90 days. Meanwhile, the application of CFSS promoted the transformation of leachable HMs into less accessible forms, which was conductive to the long-term stabilization for HMs. There was competitive relation among the three heavy metal cations, following the stabilization sequence of Cu > Zn > Cd during incubation. And the stabilization mechanisms of HMs by CFSS were proposed as chemical precipitation, surface complexation, and ion/anion exchange. The research will be greatly conducive to the remediation and governance of field multiple HMs contaminated sites.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Tongtong Zhang,Xiunan Cai,Xiangxuan Lin,Zhaoming Jiang,Hao Jin,Zuqiang Huang,Tao Gan,Huayu Hu,Yanjuan Zhang
Achieving a simultaneous increase in the redox performance of carbon nitride (CN) remains a challenge owing to the low utilization efficiency of photogenerated carriers. Herein, a novel “mechanical activation (MA)-enhanced doping and defect” strategy was proposed for structural modification of CN to enhance its performance. Specifically, CN, FeCl 3 , and thiourea were treated by MA to prepare a precursor with uniform dispersion and anchoring of Fe and S components in CN, and then the MA-treated precursor was calcinated to obtain a Fe–S co-doped CN composite (MA-Fe-S-CN) with abundant N vacancies. Under visible light illumination, MA-Fe-S-CN displayed outstanding photocatalytic performance for tetracycline (TC) removal (92.7%) and hydrogen evolution (2965 µmol g −1 h −1 ) within 120 min, which was 3.3 and 4.1 times higher than those of CN, respectively. The superlative redox performance of MA-Fe-S-CN was attributed to that MA-enhanced Fe–S co-doping and N vacancies effectively modified the built-in electric field, electronic structure, and redox potential of CN. Experimental and theoretical analysis revealed that photogenerated electrons were trapped by N vacancies and directed to Fe active sites through efficient charge transfer channels (Fe–N and Fe–S), resulting in rapid charge transfer and effective separation and utilization of carriers. On this basis, possible mechanisms of photocatalytic TC degradation and hydrogen evolution were proposed. This work provides a green and economically feasible way for improving the redox performance of CN.
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ACS Sustainable Chemistry & Engineering
·
2019
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IF 6.97
Yue Zhou,Wenhua Lv,Binglong Zhu,Fei Tong,Junli Pan,Jirong Bai,Quanfa Zhou,Hengfei Qin
Graphitic carbon nitride (g-C3N4) has been widely studied as a fascinating visible-light-response two-dimensional semiconductor photocatalyst. Nevertheless, the quantum yield of g-C3N4 is unsatisfactory due to the insufficient surface reactive sites and slow charge migration efficiency caused by grievous agglomeration and large grain size. Herein this obstacle is overcome through a facile eco-friendly strategy based on effects from a bubble template and nonmetal heteroatom doping of g-C3N4. This treatment not only restricts the agglomeration but also creates more surface active sites for reaction and more porous channels for charge carrier transfer. Well-amended g-C3N4 nanosheets with porous network and sulfur-doping were prepared with larger specific surface areas and faster electron–hole migration and separation capacity. The modified g-C3N4 nanosheets possessed a H2 evolution rate 5.3 and 3.8 times enhanced compare with bulk g-C3N4 (BCN) and S-doped g-C3N4 (CNS).
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 10
·2651-2663
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IF 5.726
Hairus Abdullah,Dong-Hau Kuo,Noto Susanto Gultom
Hydrogen-evolved Dy-doped Zn(O,S) photocatalysts with different amounts of Dy precursor have been synthesized, characterized and further utilized for hydrogenation reactions. The Dy catalysts are first examined using electrochemical impedance spectroscopy, photo responsivity, and the hydrogen evolution reaction. Dy-doped Zn(O,S) with 10% Dy precursor shows the best photocatalyst performance with the highest H2 production rate of 8.160 mmol g−1 h−1. This catalyst is chosen for conducting the hydrogenation reaction. It is our intention to confirm the correlation between the photocatalytic H2 production rate and the hydrogenation reactions of 4-nitrophenol to 4-aminophenol and azobenzene to aniline, which is a step further in the hydrogenation reaction to challenge the NN bond cleavage of azobenzene. A 100% photo conversion of 60 ppm azobenzene to aniline in 6 h was confirmed under a low-power UV light illumination in a 10% ethanol solution. Kinetic steps and kinetic mechanisms are proposed, which involve the important reaction steps of solvation, adsorption, pinning, and surface hydrogenation reaction operating together.
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