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Photoelectrocatalytic hydrogen evolution and synchronous degradation of organic pollutants by pg-C_(3)N_(4)/β-FeOOH S-scheme heterojunction

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Science China(Technological Sciences) 2024年第4期67卷 1238-1252页

作者： LI XiBao HAN Tao ZHOU YingTang XIE Yu LUO YiDan HUANG JunTong CHEN Zhi DENG Fang School of Materials Science and Engineering Nanchang Hangkong UniversityNanchang 330063China National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316022China

Crafting photoelectrocatalytic materials with robust oxidation-reduction properties for simultaneous hydrogen evolution and pollutant degradation poses a formidable challenge.In this study,a pg-C_(3)N_(4)/β-FeOOH S-scheme heterostructure with a special energy band structure was developed by anchoring porous pg-C_(3)N_(4)on needle shapedβ-FeOOH.Functioning as a hole extraction layer,needle-leaf-likeβ-FeOOH can facilitate efficient hole migration and enhance charge transport.Remarkably,the optimized 0.2-pg-C_(3)N_(4)/β-FeOOH could degrade 78%of ofloxacin(OFLO)in 90 min.The organic pollutants could absorb a large number of holes,which prompted a greater proportion of photogenerated electrons to actively participate in the hydrogen evolution reaction at the cathode.Consequently,the hydrogen production of 0.2-pg-C_(3)N_(4)/β-FeOOH reached 1452.88μmol cm^(-2)h^(-1),exhibiting a notable increase of 61.81-165.12μmol cm^(-2)h^(-1)compared with that in the absence of pollutants.Experimental and theoretical calculation results underscore that this investigation is grounded in a distinctive electron and hole dual channel transfer mechanism.These findings offer novel insights for the future development of S-scheme heterojunction photoelectrocatalytic materials capable of concurrently degrading pollutants and promoting hydrogen evolution.

关键词： photoelectrocatalysis hydrogen evolution degradation synchronous S-scheme heterojunction

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Solar-driven CO_(2) conversion to methane and methanol using different nanostructured Cu_(2)O-based catalysts modified with Au nanoparticles

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Journal of Energy Chemistry 2024年第4期91卷 287-298页

作者： João Angelo Lima Perini Lilian D.Moura Torquato Juliana Fde Brito Gustavo A.Andolpho Mateus A.Gonçalves Leonardo D.De Angelis Lucas D.Germano Susana I.Córdoba de Torresi Teodorico C.Ramalho Maria V.Boldrin Zanoni São Paulo State University(UNESP) Institute of ChemistryRua Prof.Francisco Degni55AraraquaraSP 14800-060Brazil National Institute of Alternative Technologies for Detection Toxicological Evaluation and Removal of Micropollutants and Radioactive Substances(INCT-DATREM)São Paulo State University(UNESP)Institute of ChemistryRua Prof.Francisco Degni55AraraquaraSP 14800-060Brazil Laboratory of Molecular Modelling Department of ChemistryNatural Sciences InstituteFederal University of LavrasLavrasMG 37200-900Brazil Department of Chemistry Faculty of ScienceUniversity of Hradec KrálovéHradec Králové50003Czech Republic Instituto de Química Universidade de São PauloAv.Prof.Lineu Prestes 74805508-080São PauloSPBrazil

This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator,due to itsπ-conjugated electron system.The highest production yield was achieved using a TNT@PDA/Nc/Au40%electrode,with Faradaic efficiencies of 47.4%(110.5μM cm^(-2))and 27.8%(50.4μM cm^(-2))for methanol and methane,respectively.The performance of the photoelectrodes was shown to be Cu_(2)O facet-dependent,with cubic structures leading to greater conversion of CO_(2)to methanol(43%)and methane(27%),compared to the octahedral morphology,while a higher percentage of metallic gold on the nanostructured Cu_(2)O surface was mainly important for CH4production.Density functional theory(DFT)calculations supported these findings,attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40%electrode for CH4generation to the formation of an OCH3intermediate bonded to Au atoms.Studies using isotope-labeling and analysis by gas chromatograph-mass(GC-MS)demonstrated that13CO_(2)was the source for photoelectrocatalytic generation of13CH3OH and13CH313CH2OH.

关键词： Cu_(2)O nanocubes photoelectrocatalysis Polydopamine CO_(2) photoelectroreduction DFT calculations

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Recent progress in photoelectrocatalysis of g-C3N4 for water environment remediation

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Progress in Natural Science:Materials International 2022年第5期32卷 538-553页

作者： Fenfen Liang Huifang Wang Ruoqi Yu Cheng Liu Yali Wang Lizhong Bai Chunli Hao Guodong Hao The Cultivation Base of Shanxi Key Laboratory of Mining Area Ecological Restoration and Solid Wastes Utilization Shanxi Institute of Technology Department of Materials Science and Engineering Shanxi Institute of Technology Mudanjiang Normal University

Water environmental pollutants have become one of the most serious environmental issues, and the removal of various environmental pollution(dyes, phenols, pesticides, heavy metal ions, etc.) is of particular concern because of their toxicity and refractory. Compared to conventional eliminating routes, photoelectrocatalysis(PEC), is considered as a promising strategy since it combines the advantages of photocatalysis(PC) and electrocatalysis(EC). However, it still encounters bottlenecks of scarce reaction sites and low product selectivity, restricting its development toward practical applications. In recent years, various of g–C3N4–based composites were used for the remediation of these typical environmental pollutants. Given this situation, this review summarizes the latest progress in the design and preparation of novel g–C3N4–based composites and their PEC degradation different pollution in the water environment. Some removal mechanisms are briefly discussed, and the prospects are presented for further research.

关键词： photoelectrocatalysis G-C 3 N 4 Pollutants removal Water environment

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Flexible hollow TiO_(2)@CMS/carbon-fiber van der Waals heterostructures for simulated-solar light photocatalysis and photoelectrocatalysis

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Journal of Materials Science & Technology 2022年第3期98卷 143-150页

作者： Hua-Jun Chen Yan-Ling Yang Xin-Xin Zou Xiao-Lei Shi Zhi-Gang Chen School of Materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China School of Environment and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471000China Centre for Future Materials University of Southern QueenslandSpringfield CentralQLD 4300Australia School of Mechanical and Mining Engineering The University of QueenslandBrisbaneQLD 4072Australia

The recycling technology of photocatalyst powdery has hardly been mature in the photocatalytic oxidation so far.In this work,the hollow TiO_(2)microspheres with an appropriate thickness are confined in carbon microspheres(CMSs)to form hollow TiO_(2)@CMSs,which are physically integrated with carbon-fiber textile by van der Waals(vdW)interactions to generate separable and recyclable hollow TiO_(2)@CMSs/carbon-fiber vdW heterostructures.Such separable and recyclable heterostructures show remarkable oxidation of 2,4-dinitrophenol.From our detailed characterization and density functional theory(DFT)calculations,we found that carbon fiber can trap electrons exerted from the excitation of hollow TiO_(2)@CMSs and creates holes in hollow TiO_(2)microspheres,which endow the carbon fiber with photocatalytic activity through coherent charge injection.This study indicates that our general strategy for the fabrication of hollow TiO_(2)@CMSs/carbon-fiber vdW heterostructures can be used as separable and recyclable photocatalyst and photoelectrocatalyst with potential industrial applications in environmentrelated fields.

关键词： Hollow nanostructure TiO_(2) Carbon fiber van der Waals heterostructure photoelectrocatalysis

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Peroxymonosulfate enhanced photoelectrocatalytic oxidation of organic contaminants and simultaneously cathodic recycling of silver

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Journal of Environmental Sciences 2022年第10期34卷 74-83页

作者： Huixin Shao Xia Li Juanjuan Zhang Xu Zhao Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Beijing Capital Co.Ltd. Beijing 100028China

Degradation of organic contaminants with simultaneous recycling of Ag+from silvercontaining organic wastewater such as photographic effluents is desired. Although photoelectrocatalysis(PEC) technology is a good candidate for this type of wastewater, its reaction kinetics still needs to be improved. Herein, peroxymonosulfate(PMS) was employed to enhance the PEC kinetics for oxidation of phenol(PhOH) at the anode and reduction of Ag^(+) at the cathode. The degradation efficiency of phenol(PhOH, 0.1 mmol/L) was increased from 42.8% to 96.9% by adding 5 mmol/L PMS at a potential of 0.25 V. Meanwhile, the Ag(by wt%)deposited on the cathode was 28.1%(Ag_(2)O) in PEC process, while that of Ag(by wt%) was 69.7%(Ag^(0)) by adding PMS. According to the electrochemistry analysis, PMS, as photoelectrons acceptor, enhances the separation efficiency of charges and the direct hoxidation of Ph OH at the photoanode. Meantime, the increasing cathode potential avoided Hevolution and strongly alkaline at the surface of cathode, thus enabling the deposition of Ag+in the form of metallic silver with the help of PMS. In addition, PMS combined with PEC process was effective in treating photographic effluents.

关键词： Peroxymonosulfate photoelectrocatalysis Organic contaminants degradation Silver recycling Photographic effluents

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Surface amorphization oxygen vacancy-rich porous Sn_(3)O_(x)nanosheets for boosted photoelectrocatalytic bacterial inactivation

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Rare Metals 2023年第5期42卷 1508-1515页

作者： Long-Wei Wang Lin Liu Zhen You Li-Wei Zhang Xiao-Di Zhang Na Ren Hong Liu Xin Yu Institute for Advanced Interdisciplinary Research(iAIR) School of Chemistry and Chemical EngineeringUniversity of JinanJinan250022China Key Laboratory of Resource Biology and Biotechnology in Western China Ministry of Education School of MedicineNorthwest UniversityXi’an710069China Institute for Cell Engineering Department of NeurologyJohns Hopkins University School of MedicineBaltimoreMD21205USA State Key Laboratory of Crystal Material Shandong UniversityJinan250100China

Antibiotic misuse has resulted in the emergence of superbugs,warranting new antibacterial methods.Surface amorphisation oxygen vacancy-rich porous Sn_(3)O_(x)nanosheets in situ grown on Ni foam are successfully designed via a simple,one-step hydrothermal method,resulting in enhanced photoelectrochemical(PEC)bacterial inactivation.In this system,the porous structure enriches its surface with oxygen vacancies,which can extend the absorption spectrum into the near-infrared region,while oxygen vacancies can enhance the separation of electronhole pairs.Most importantly,the sheet-like porous structure enhances surface active sites and increase the contact area between bacteria and electrodes.Therefore,the reactive oxygen species produced during the PEC process can directly act on the surface of bacteria and is100%effectively against drug-resistant Gram-positive and Gram-negative bacteria in water within 30 min.This study acts as a foundation for the development of novel photoelectrocatalyst electrodes for efficient water purification.

关键词： Oxygen vacancy photoelectrocatalysis Water purification Sn_(3)O_(x) Bacterial killing

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Defect-designed Mo-doped BiVO_(4)photoanode for efficient photoelectrochemical degradation of phenol

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Journal of Materials Science & Technology 2023年第34期165卷 225-234页

作者： Mufeng Yu Yiming Tang Yuxin Liao Wanhan He Xin-xin Lu Xin Li School of Environment Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety&MOE Key Laboratory of Theoretical Chemistry of EnvironmentSouth China Normal UniversityGuangzhou 510006China PetroChina Shenzhen New Energy Research Institute Shenzhen 518052China Institute of Biomass Engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

The monoclinic scheelite BiVO_(4)has impressive properties such as a narrow energy band gap,exceptional stability,and extended absorption in visible light,making it a suitable photoanode.Nevertheless,the BiVO_(4)material encounters challenges such as the high recombination rate of photogenerated electronhole pairs and poor photoelectron conductivity,which limits photocatalytic activity.To address this problem,we developed Mo-doped BiVO_(4)films on FTO substrates for photoelectrocatalytic degradation of phenol.When exposed to visible light,the Mo-BiVO_(4)film attained a 70%degradation of phenol in 120 min with a 1.2 V vs.Ag/AgCl bias—a 3.7 times improvement from pristine BiVO_(4).Mo-doping facilitates better migration and separation of electron-hole pairs and increases the concentration of photogenerated carriers,leading to an upward shift of the valence band potential direction,and an improvement in oxidation capacity.Furthermore,density-functional theory(DFT)calculations were used to explain how Modoping with BiVO_(4)improves the adsorption energy to phenol degradation intermediates,emphasizing its effectiveness in promoting phenol degradation.Therefore,with the inclusion of DFT calculations,this work provides a more comprehensive understanding of the mechanism underlying the enhancement of photocatalytic activity by Mo-doped BiVO_(4),which is crucial information for the further development of effective and efficient photoanodes.

关键词： BiVO_(4) Doping photoelectrocatalysis Phenol DFT calculations

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Photoelectrocatalytic principles for meaningfully studying photocatalyst properties and photocatalysis processes:From fundamental theory to environmental applications

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Journal of Energy Chemistry 2023年第11期86卷 84-117,I0003页

作者： Jiafang Liu Shengbo Zhang Weikang Wang Haimin Zhang Key Laboratory of Materials Physics Centre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei 230031AnhuiChina University of Science and Technology of China Hefei 230026AnhuiChina School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina

Photocatalysis is critically important for environmental remediation and renewable energy technologies.The ability to objectively characterize photocatalyst properties and photocatalysis processes is paramount for meaningful performance evaluation and fundamental studies to guide the design and development of high-performance photocatalysts and photocatalysis systems.Photocatalysis is essentially an electron transfer process,and photoelectrocatalysis(PEC)principles can be used to directly quantify transferred electrons to determine the intrinsic properties of photocatalysts and photocatalysis processes in isolation,without interference from counter reactions due to physically separated oxidation and reduction half-reactions.In this review,we discuss emphatically the PEC-based principles for characterizing intrinsic properties of photocatalysts and important processes of photocatalysis,with a particular focus on their environmental applications in the degradation of pollutants,disinfection,and detection of chemical oxygen demand(COD).An outlook towards the potential applications of PEC technique is given.

关键词： photoelectrocatalysis Photocatalytic intrinsic properties Photocatalytic characterization Environmental remediation photoelectrocatalysis-based application

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A review on photo-, electro- and photoelectro- catalytic strategies for selective oxidation of alcohols

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Journal of Energy Chemistry 2023年第2期77卷 80-118,I0003页

作者： Duoyue Tang Guilong Lu Zewen Shen Yezi Hu Ling Yao Bingfeng Li Guixia Zhao Baoxiang Peng Xiubing Huang MOE Key Laboratory of Resources and Environmental System Optimization College of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China Laboratory of Industrial Chemistry Ruhr University Bochum44780 BochumGermany POWERCHINA SICHUN Electric Power Engineering CO. LTDChengdu 610041SichuanChina Beijing Key Laboratory of Function Materials for Molecule&Structure Construction School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Traditional conversion of alcohols into carbonyl compounds exists a few drawbacks such as harsh reaction conditions,production of large amounts of hazardous wastes,and poor selectivity.The newly emerging conversion approaches via photo-,electro-,and photoelectro-catalysis to oxidize alcohols into high value-added corresponding carbonyl compounds as well as the possible simultaneous production of clean fuel hydrogen(H_(2))under mild conditions are promising to substitute the traditional approach to form greener and sustainable reaction systems and thus have aroused tremendous investigations.In this review,the state-of-the-art photocatalytic,electrocatalytic,and photoelectrocatalytic strategies for selective oxidation of different types of alcohols(aromatic and aliphatic alcohols,single alcohol,and polyols,etc.)as well as the simultaneous production of H_(2) in certain systems are discussed.The design of photocatalysts,electrocatalysts,and photoelectrocatalysts as well as reaction mechanism is summarized and discussed in detail.In the end,current challenges and future research directions are proposed.It is expected that this review will not only deepen the understanding of environmentally friendly catalytic systems for alcohol conversion as well as H_(2) production,but also enlighten significance and inspirations for the follow-up study of selective oxidation of various types of organic molecules to value-added chemicals.

关键词： Alcohol oxidation Carbonyl compounds Photocatalysis Electrocatalysis photoelectrocatalysis

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Solar-driven green synthesis of epoxides

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Science China Chemistry 2023年第12期66卷 3415-3425页

作者： Daojian Tang Kun Dang Jiaming Wang Chuncheng Chen Jincai Zhao Yuchao Zhang Key Laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Epoxides are one of the most important intermediates used in the production of valuable chemicals. Traditional preparation methods often rely on hazardous oxidants or extensive fossil fuel-powered thermal catalytic systems, resulting in significant waste production and CO_(2) emissions. Solar-driven photo(electro)chemistry is an emerging option for achieving the environmentally-friendly synthesis of epoxides. In this review, we firstly summarize the fundamental understanding of epoxidation reactions among various systems, including molecular catalysis, heterogeneous thermal catalysis and electrocatalysis. Then, we focus on the recent advances in the synthesis of epoxides achieved by photo(electro)chemical approaches. This review is concluded by the rational design of photoelectrochemical systems towards efficient epoxide synthesis.

关键词： olefin epoxidation solar energy conversion plasmonic catalysis photoelectrocatalysis oxygen atom transfer

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