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Shedding light on the role of interfacial chemical bond in heterojunction photocatalysis

Nano Research 2022年第12期15卷 10158-10170页

作者： Yueshuang Mao Pengfei Wang sihui zhan MOE Key Laboratory of Pollution Processes and Environmental Criteria College of Environmental Science and EngineeringNankai UniversityTianjin300350China Tianjin Key Lab Clean Energy&Pollutant Control School of Energy and Environmental EngineeringHebei University of TechnologyTianjin300401China

Faced with the growing consumption of fossil fuels and the consequent energy/ecological crisis,photocatalysis has become a realistic option to develop new energy source and realize the carbon *** photocatalysts constructed by multiple semiconductors with staggered band structure can spatially separate redox reaction sites to realize synergistic oxidation and reduction reactions,and have captured broad ***,the undesigned heterojunctions still encounter some headache difficulties,that is the poor interfacial contact,which will block carrier mobility,thus result in inefficient and instable ***,researchers have been focusing on constructing chemical bonds(especially covalent bonding)between different semiconductors to induce the formation of intimate and stable interface ***,this review article presents the state-of-the-art progress on interfacial chemical bonds(ICB)in heterojunction photocatalysts and clarifies the function mechanism for enhancing *** that the formation of ICB strongly depends on the surface characteristics of semiconductors,we clarify the formation mechanism and put forward rational design *** importantly,the current photocatalytic applications of ICB are reviewed to have a deep understanding of structure-activity related ***,our brief outlooks on the current challenges and future development trends of ICB for next-generation photocatalysts are pointed out to create brand-new strategies for optimizing photocatalytic properties and accelerate the practical applications of ICB with high-performance.

关键词： photocatalysis heterojunction interfacial chemical bond structure-activity relationships charge transfer

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Efficient removal for multiple pollutants via Ag_(2)O/BiOBr heterojunction:A promoted photocatalytic process by valid electron transfer pathway

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Chinese Chemical Letters 2020年第10期31卷 2698-2704页

作者： Zhiruo Zhou Yanan Li Mingmei Li Yi Li sihui zhan College of Environmental Science and Engineering Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300071China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin 300072China Tianjin Key Lab for Rare Earth Materials and Applications Tianjin 300072China

Multiple pollutants including pathogenic microorganism contaminations and emerging organic contaminations(EOCs)have shown a growing threat to the environment,especially the natural ***,the control and removal of pathogenic microorganism contaminations and EOCs have been greatly limited since limited knowledge of their environmental ***,a novel and efficient photocatalyst Ag_(2)O/BiOBr heterojunction was synthesized and used for removal of multiple pollutants including Escherichia coli(***),Staphylococcus aureus(***),tetracycline and acetaminophen under visible *** results showed that there were valid electron transfer pathways between BiOBr and Ag_(2)O,the main electron transfer direction was the BiOBr to Ag_(2)***-generated electrons were stored in Ag_(2)O and thus separation efficiency between holes and photo-generated electrons was obviously *** oxygen species were highly produced and eventually end up with the high efficiency of removal of multiple *** Ag_(2)O/BiOBr with Ag_(2)O content at 3%(the best performance)under visible light,log decrease of *** was 7.16(removal efficiency was 100%)in 120 min,log decrease of *** was 7.23(removal efficiency was 100%)in 160 min,C/C0 of tetracycline was 0.06 in 180 min,C/C0 of acetaminophen was 0.17 in 180 *** work could provide a promising candidate in the actual contaminated natural waters for cleaning multiple pollutants.

关键词： Water pollution Photocatalysis Multiple pollutants Electrons transfer channels

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Towards single-atom photocatalysts for future carbon-neutral application

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SmartMat 2022年第3期3卷 417-446页

作者： Dongpeng zhang Yanxiao Li Yi Li sihui zhan MOE Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlCollege of Environmental Science and EngineeringNankai UniversityTianjinChina Department of Chemistry Tianjin UniversityTianjinChina

The implementation of carbon neutrality to achieve the goal of controlling global warming in the Paris Climate Agreement is currently the most important international climate *** utilization of solar energy through photocatalysts is of great significance to the adjustment of energy ***-atom photocatalysts have excellent catalytic activity and selectivity in a variety of applications,including sustainable energy conversion,chemical synthesis,CO_(2)reduction,environmental remediation,and other areas,owing to their unique electronic structure and high atom ***,we elaborated on the content and implementation direction of the carbon neutrality policy and demonstrated the design principles of single-atom *** single-atom synthesis strategies are summarized,and representative characterization methods have been shown to further reveal the structure–performance ***,we focus on the application of single-atom photocatalysts in CO_(2)reduction,sustainable energy conversion,and environmental ***,the opportunities and challenges in the application of single-atom photocatalysts were discussed based on its current development.

关键词： carbon neutrality CO_(2)reduction hydrogen photocatalysts single-atom catalysts synthesis strategies

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Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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Science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao sihui zhan MOE Key Laboratory of Pollution Processes and Environmental Criteria/Tianjin Key Laboratory of Environmental Remediation and Pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen ***,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major ***,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/*** feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom *** article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting *** article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

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Cobalt diselenide (001) surface with short-range Co-Co interaction triggering high-performance electrocatalytic oxygen evolution

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Nano Research 2021年第12期14卷 4848-4856页

作者： Kun Dang Shihao zhang Xuewei Wang Wenming Sun Ligang Wang Yang Tian sihui zhan Department of Chemistry Analytical Instrumentation CenterBeijing Key Laboratory for Optical Materials and Photonic DevicesCapital Normal UniversityBeijing100048China MOE Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlCollege of Environmental Science and EngineeringNankai UniversityTianjin300350China College of Science China Agricultural UniversityBeijing100193China Beijing National Laboratory for Molecular Sciences(BNLMS) College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

Oxygen evolution reaction (OER) still suffers from the bottleneck in electrocatalytic water splitting. Herein, in virtue of volcano plots drawn by theoretical calculation, the (001) facet was screened as the superb facet of orthorhombic CoSe_(2) for OER. Afterwards, CoSe_(2)(001) nanosheets were synthesized and the exposure ratio of (001) facet is controllable with thermodynamics methods effectively. The single-facet CoSe2(001) delivered an overpotential as low as 240 mV at 10 mA·cm^(−2) in 1 M KOH, which outperformed the bulk (380 mV) as well as other CoSe_(2)-base OER catalysts reported before. Especially, a shorter Co-Co path was observed in CoSe_(2)(001) by X-ray absorption spectroscopy. Further density functional theory (DFT) studies revealed that the reversible compression on the shorter Co-Co path could regulate the electronic structure of active sites during the OER process, and thus the energy barrier of the rate-determining step was reduced by 0.15 eV. This work could inspire more insights on the modification of electronic structure for OER electrocatalysts.

关键词： CoSe2 oxygen evolution reaction(OER) water-splitting electrocatalysis crystal facet engineering electronic structure manipulation

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A Unifi ed View of Carbon Neutrality:Solar-Driven Selective Upcycling of Waste Plastics

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Transactions of Tianjin University 2024年第1期30卷 1-26页

作者： Zhiyong Zhao Shuai Yue Gaohua Yang Pengfei Wang sihui zhan MOE Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlCollege of Environmental Science and EngineeringTianjin 300350China

With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental *** the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and *** can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon *** this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added ***,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.

关键词： Photocatalysis Photoreforming Plastics upcycling Carbon neutrality Energy storage and conversion

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Simulated-sunlight-activated photocatalysis of Methylene Blue using cerium-doped SiO_2/TiO_2 nanostructured fibers

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Journal of Environmental Sciences 2012年第10期24卷 1867-1875页

作者： Yu Liu Hongbing Yu Zhenning Lv sihui zhan Jiangyao Yang Xinhong Peng Yixuan Ren Xiaoyan Wu College of Environmental Science and Engineering Nankai UniversityT'wnjin 300071China

Cerium-doped SiO2/TiO2 nanostructured fibers were fabricated by electrospinning technology. The prepared fibers were characterized by thermogravimetric analysis （TGA）, scanning electron microscopy （SEM）, X-ray diffraction （XRD） and Fourier transform infrared spectroscopy （FT-IR）. Using the fibers as catalysts, photoeatalytic degradation of Methylene Blue （MB） aqueous solution was carded out under simulated sunlight. The 0.2% Ce doping proved to be the optimal concentration for the doping of TiO2/SiO2, compared to other Ce-doped molar concentrations. The 0.2% Ce-doped SiOdTiO2 fibers exhibited higher photocatalytic activity than industrial Degussa P25 and the samples doped with only Ce or SIO2. The reasons for improving the photocatalytic activity were also discussed. Several operational parameters were studied, which showed that the photocatalytic efficiency of MB was influenced by parameters such as the initial dye concentration, the initial pH, inorganic anions, and so on. In addition, the influences of an electron acceptor and a radical scavenger suggested that OH was the dominant photooxidant during the photocatalytic process. The reuse evaluation of the fibers indicated that their photocatalytic activity had good stability.

关键词： photocatalysis SiO2/TiO2 cerium nanostructured fibers Methylene Blue

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Construction of Z-scheme Cu-CeO_(2)/BiOBr heterojunction for enhanced photocatalytic degradation of sulfathiazole

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Chinese Chemical Letters 2024年第7期35卷 167-172页

作者： Xingmin Chen Yunyun Wu Yao Tang Peishen Li Shuai Gao Qiang Wang Wen Liu sihui zhan College of Environmental Sciences and Engineering Nankai UniversityTianjin 300350China Laboratory for Micro-Sized Functional Materials&College of Elementary Education and Department of Chemistry Capital Normal UniversityBeijing 100048China College of Environmental Sciences and Engineering The Key Laboratory of Water and Sediment Sciences(MOE)Peking UniversityBeijing 100871China

The utilization of an efficient photocatalyst is crucial for the photocatalytic degradation of antibiotics in water through visible light,which is an imperative requirement for the remediation of water *** this study,a novel Cu-CeO_(2)/BiOBr Z-type heterojunction was synthesized by calcination and hydrothermal methods,and the degradation rate of sulfathiazole(STZ)antibiotic solution was studied using simulated illumination(300 W xenon lamp).The results indicated that 3%Cu-CeO_(2)/BiOBr achieved a degradation rate of 92.3%within 90 min when treating 20 mg/L STZ solution,demonstrating its potential for practical water treatment *** using various chemical instruments revealed that 3%Cu-CeO_(2)/Bi OBr exhibited the lowest electron-hole recombination rate and electron transfer ***,the utilization of ESR data and quenching experiments has substantiated the involvement of hydroxyl radicals(·OH)and superoxide radicals(·O_(2)^(-))as the primary active ***,a plausible degradation mechanism has been *** findings offer a prospective approach for the development of heterojunction materials with appropriate band matching.

关键词： Cu-CeO_(2)/BiOBr nanoheterojunction Photocatalytic degradation Sulfathiazole Z-scheme

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In situ integration of efficient photocatalyst Cu1.8S/ZnxCd1-xS heterojunction derived from a metal-organic framework

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Chinese Chemical Letters 2020年第10期31卷 2795-2798页

作者： Dongpeng zhang Pengfei Wang Fangyuan Chen Kelei Mu Yi Li Haitao Wang Zhijun Ren sihui zhan MOE Key Laboratory of Pollution Processes and Environmental Criteria/Tianjin Key Laboratory of Environmental Remediation and Pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China School of Energy and Environmental Engineering Hebei University of TechnologyTianjin 300401China Department of Chemistry Tianjin UniversityTianjin 300072China

The development of photocatalysts for hydrogen evolution is a promising alternative to industrial hydrogen evolution;however,generation of high active,recyclable,inexpensive heterojunctions are still ***,a novel strategy was developed to synthesize non-noble metal co-catalyst/solid solution heterojunctions using metal-organic frameworks(MOFs)as a precursor *** adjusting the content of MOFs,a series of Cu1.8S/ZnxCd1-xS heterojunctions were obtained,and the Cu1.8S(3.7%)/Zn0.35Cd0.65S sample exhibits a maximum hydrogen evolution rate of 14.27 mmol h^(-1) g^(-1) with an apparent quantum yield of 3.7%at 420 nm under visible-light ***,the relationship between the heterojunction and photocatalytic activity were investigated by detailed characterizations and density functional theory(DFT)calculations,which reveal that loading Cu1.8S can efficiently extend the light absorption,meanwhile,the electrons can efficiently transfer from Zn0.35Cd0.65S to Cu1.8S,thus resulting more photogenerated electrons participating in surface *** result can be valuable inspirations for the exploitation of advanced materials using rationally designed nanostructures for solar energy conversion.

关键词： Co-catalyst Cu1.8S/Zn0.35Cd0.65S Density functional theory(DFT) Charge separation and transfer

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Inorganic Ultrathin 2D Photocatalysts:Modulation Strategies and Environmental/Energy Applications

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Accounts of Materials Research 2023年第1期4卷 4-15页

作者： Mingmei Li He zhang Zhiyong Zhao Pengfei Wang Yi Li sihui zhan MOE Key Laboratory of Pollution Processes and Environmental Criteria College of Environmental Science and EngineeringNankai UniversityTianjin 300350China Tianjin Key Lab Clean Energy&Pollutant Control School of Energy and Environmental EngineeringHebei University of TechnologyTianjin 300401China

CONSPECTUS:Photocatalysis technology has gained extensive attention in the past few decades due to its potential to alleviate or solve energy and environmental contamination *** development and design of new photocatalytic semiconductor materials with high catalytic activity has become a research hotspot in this *** recent years,inorganic ultrathin two-dimensional(2D)semiconductor photocatalysts have shown excellent performance in photocatalytic applications due to their high specific surface area,clear atomic structure,unique electronic structure,intrinsic quantum confined electrons,and high atomic exposure *** the thickness of the bulk semiconductor is decreased to the atomic level,its local atomic structure changes *** is a major reason why the atomic thin 2D materials could show improved inherent properties and produce new properties that are not available in the corresponding bulk ***,compared with the bulk photocatalysts,the surface electronic structure of inorganic ultrathin 2D materials is more sensitive and thus could be regulated more easily by surface and interfacial modification methods,leading to great optimization of photocatalytic ***,inorganic ultrathin 2D materials not only provide an ideal reaction model for clearly revealing the relationships between surface/interface structure characteristics and photocatalytic performance but also bring new opportunities for the development of efficient catalysts to resolve energy crises and environmental *** this Account,we summarize our previous work on the applications of inorganic ultrathin 2D nanomaterials in the field of ***,we briefly introduce the classification and controlled fabrication of inorganic ultrathin 2D nanomaterials,including metal chalcogenides,bismuth-based photocatalysts,metal oxides,and metal-free ***,we focus on the surface and interfacial modification strategies for effectively

关键词： inorganic thin Photo

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