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Probing of coupling effect induced plasmonic charge accumulation for water oxidation

National Science Review 2021年第6期8卷 160-168页

作者： Yuying Gao Feng Cheng Weina Fang Xiaoguo Liu Shengyang Wang Wei Nie Ruotian Chen Sheng Ye Jian Zhu Hongyu An Chunhai Fan Fengtao Fan Can Li State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy Materials (i Ch EM)Dalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences School of Chemistry and Chemical Engineering and Institute of Molecular MedicineRenji HospitalSchool of MedicineShanghai Jiao Tong University

A key issue for redox reactions in plasmon-induced photocatalysis, particularly for water oxidation, is the concentration of surface-accumulating charges(electrons or holes) at a reaction site for artificial photosynthesis. However, where plasmonic charge accumulated at a catalyst’s surface, and how to improve local charge density at active sites, remains unknown because it is difficult to identify the exact spatial location and local density of the plasmon-induced charge, particularly with regard to holes. Herein, we show that at the single particle level, plasmon-coupling-induced holes can be greatly accumulated at the plasmonic Au nanoparticle dimer/Ti O2 interface in the nanogap region, as directly evidenced by the locally enhanced surface photovoltage. Such an accumulation of plasmonic holes can significantly accelerate the water oxidation reaction(multi-holes involved) at the interfacial reaction site, with nearly one order of magnitude enhancement in photocatalytic activities compared to those of highly dispersed Au nanoparticles on Ti O2. Combining Kelvin probe force microscopy and theoretical simulation, we further clarified that the local accumulated hole density is proportional to the square of the local near-field enhancement. Our findings advance the understanding of how charges spatially distribute in plasmonic systems and the specific role that local charge density at reaction sites plays in plasmonic photocatalysis.

关键词： plasmonic photocatalysis coupling effect Charge separation surface photovoltage spatial distribution

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Preparation of Bi_(2)O_(3)/BiOI Step-scheme Heterojunction Photocatalysts and Their Degradation Mechanism of Methylene Blue

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Journal of Wuhan University of Technology(Materials Science) 2022年第5期37卷 801-806页

作者：姜雪超谭海燕 SHI Xinyu CHENG Xinhua HU Weibing HU Xinhui Key Laboratory of Green Manufacturing of Super-light Elastomer Materials of State Ethnic Affairs Commission School of Chemistry and Environmental EngineeringHubei Minzu UniversityEnshi445000China Guangxi Key Laboratory of Chemistry and Engineering of Forest Products Guangxi University for NationalitiesNanning530006China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China

Bi_(2)O_(3)/BiOI step-scheme(S-scheme) heterojunction photocatalyst was synthesized by green calcination method, its degradation ability of methylene blue was investigated, and the photocatalytic performance of the Bi_(2)O_(3)/BiOI heterojunction, Bi_(2)O_(3) and BiOI was compared. The structure and morphology of the samples were characterized by X-ray diffraction(XRD), field emission scanning electron microscopy(FESEM), and UV-vis diffuse reflection spectrum (UV-vis DRS). The degradation rate of methylene blue was analysised by spectrophotometry, and the calculation result showed that the degradation rate of methylene blue was 97.8% in 150 minutes. The first order kinetic rate constant of 10%Bi_(2)O_(3)/BiOI is 0.021 8 min^(-1), which are2.37 and 2.68 times of BiOI(0.009 18 min^(-1)) and Bi_(2)O_(3) (0.008 03 min^(-1)) respectively. The calculation result shows that the work function of Bi_(2)O_(3) and BiOI are 3.0 e V and 6.0 e V, respectively, by density functional theory(DFT). When this S-scheme heterojunction is used as a photocatalyst, the weaker electrons in the conduction band of BiOI will be combined with the weaker holes in the Bi_(2)O_(3) valence band under combined effect with built-in electric field and band bending, which will retain stronger photoelectrons and holes between Bi_(2)O_(3) and BiOI. This may be the internal reason for the efficient degradation of tetracycline by Bi_(2)O_(3)/BiOI S-scheme heterostructures.

关键词： step-scheme heterojunction methylene blue antibiotic wastewater treatment photocatalytic degradation Charge separation

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Achieving an electron transfer photochromic complex for switchable white-light emission

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Chinese Chemical Letters 2022年第6期33卷 3203-3206页

作者： Qi Li Wuji Wei Zhenzhen Xue Ying Mu Jie Pan Jixiang Hu Guoming Wang College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China

Tuning white-light emission via free radicals is still a challenge in molecular-based functional materials.Herein, a new photoactive Zn^(2+) oxalate-based chain containing a polypyridine ligand was designed and synthesized with remarkably bifunctional photochromism and photo-actuated greenish white-light emission after UV, sunlight or Xe lamp light irradiation at room temperature. The photo-actuated coloration process was induced by the photogeneration of stable radicals originated from intermolecular electron transfers from oxalate components to the protonated polypyridine units, as demonstrated by UV–vis, IR,electron spin resonance and X-ray photoelectron spectra and magnetic measurements. Importantly, the on/off greenish white light emission(WLE) could be reversibly switched by generation and elimination of radicals via light irradiation and heat treatment, providing a feasible strategy for designing photoswitchable light emission diodes materials.

关键词： Charge separation Electron transfer Photochromism Photogenerated radicals White-light emission

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Construction of immobilized films photocatalysts with CdS clusters decorated by metal Cd and BiOCl for photocatalytic degradation of tetracycline antibiotics

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Chinese Chemical Letters 2022年第8期33卷 3705-3708页

作者： Jiajia Li Ziwei Zhao Zhuoning Li Huijuan Yang Shijun Yue Yuping Tang Qizhao Wang Key Laboratory of Shaanxi Administration of Traditional Chinese Medicine for TCM Compatibility and State Key Laboratory of Research&Development of Characteristic Qin Medicine Resources(Cultivation)and Shaanxi Key Laboratory of Chinese Medicine Fundamentals and New Drugs Researchand Shaanxi Collaborative Innovation Center of Chinese Medicinal Resources IndustrializationShaanxi University of Chinese MedicineXianyang 712046China School of Water and Environment Chang'an UniversityXi'an 710064China College of Chemistry and Chemical Engineering Northwest Normal UniversityLanzhou 730070China Institute of Advanced Electrochemical Energy School of Materials Science and Engineering Xi'an University of Technologyand Shaanxi International Joint Research Centre of Surface Technology for Energy Storage MaterialsXi'an 710048China

A kind of CdS/Cd-BiOCl immobilized films photocatalyst was prepared.The optical and physicochemical properties of the CdS/Cd-BiOCl photocatalysts were analysed,and the detailed characterization revealed CdS/Cd-BiOCl films photocatalyst with good charge carrier separation effect.The reusabilities and photocatalytic properties of the samples were studied.The 15%Cd S/Cd-Bi OCl photocatalyst exhibited superior performance in photocatalytic degradation of tetracycline(TC)and favorable stability under visible light irradiation.As for the photodegradation rate of TC,15%CdS/Cd-BiOCl exhibited an excellent photodegradation activity,which is 4.06 and 9.53 times higher than that of Cd S/Cd and Bi OCl,respectively.The results showed that dominant active species are·O_(2)^(-)and·OH radicals during photodegradation.The charge transfer in Z-scheme CdS/Cd-BiOCl films photocatalyst could synchronously generate conduct band(CB)electrons in BiOCl and valence band(VB)holes in CdS,and metal Cd served as electron mediator.This work can be a reference for the design of film photocatalysts and new insight for photodegradating towards contaminants.

关键词： CdS/Cd-BiOCl immobilized films photocatalyst Photodegradation mechanism Environmental remediation Charge separation Tetracycline

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Photo-piezoelectric synergistic degradation of typical volatile organic compounds on BaTiO_(3)

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Chinese Chemical Letters 2022年第1期33卷 410-414页

作者： Qin Liu Weina Zhao Zhimin Ao Taicheng An Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China

Explore the photo-piezoelectric synergistic micro-mechanism by density functional theory(DFT)calculations at the electronic and atomic level is important.In this work,to understand the synergistic mechanism,atomic and electronic properties of typical piezoelectric and photocatalytic material BaTiO_(3)were initially investigated with different strains.Subsequently,the adsorption of volatile organic compounds(VOCs)on the BaTiO_(3)(001)surface was determined during the piezoelectric process.In addition,the relationship between deformation ratio,the electronic structure and adsorption energy was understood in the deformation ratio range of 7%-12%for the optimal catalytic effect.The results of charge density differences and Born effective charge reveal the synergistic mechanism of piezoelectric photocatalysis.The built-in electric field formed by polarization results in the enhanced separation of charges,which makes the surface charges aggregation,enhancing the adsorption of VOCs,and benefiting the subsequent photocatalytic degradation.This work can provide significant theoretical guidance for the piezoelectric photocatalytic degradation of pollutants with the optimal strain range.

关键词： Photocatalysis Photo-piezoelectric synergistic Polarization Charge separation BaTiO_(3) Volatile organic compounds(VOCs)

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Experimental and DFT Studies of Au Deposition Over WO_(3)/g-C_(3)N_(4) Z-Scheme Heterojunction

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Nano-Micro Letters 2020年第1期12卷 75-92页

作者： Muhammad Humayun Habib Ullah Junhao Cao Wenbo Pi Yang Yuan Sher Ali Asif Ali Tahir Pang Yue Abbas Khan Zhiping Zheng Qiuyun Fu Wei Luo Engineering Research Center for Functional Ceramics of the Ministry of Education School of Optical and Electronic InformationHuazhong University of Science and TechnologyWuhan 430074People’s Republic of China China‑EU Institute for Clean and Renewable Energy Huazhong University of Science and TechnologyWuhan 430074People’s Republic of China Environment and Sustainability Institute(ESI) University of ExeterPenryn CampusPenrynCornwall TR109FEUK College of Engineering and Applied Sciences Nanjing UniversityNanjing 210093People’s Republic of China Department of Chemistry Abdul Wali Khan UniversityMardanKhyber Pakhtunkhwa 23200Pakistan

A typical Z-scheme system is composed of two photocatalysts which generate two sets of charge carriers and split water into H2 and O2 at different locations.Scientists are struggling to enhance the efficiencies of these systems by maximizing their light absorption,engineering more stable redox couples,and discovering new O2 and H2 evolutions co-catalysts.In this work,Au decorated WO3/g-C3N4 Z-scheme nanocomposites are fabricated via wet-chemical and photo-deposition methods.The nanocomposites are utilized in photocatalysis for H2 production and 2,4-dichlorophenol(2,4-DCP)degradation.It is investigated that the optimized 4Au/6%WO3/CN nanocomposite is highly efficient for production of 69.9 and 307.3μmol h−1 g−1 H2 gas,respectively,under visible-light(λ>420 nm)and UV–visible illumination.Further,the fabricated 4Au/6%WO3/CN nanocomposite is significant(i.e.,100%degradation in 2 h)for 2,4-DCP degradation under visible light and highly stable in photocatalysis.A significant 4.17%quantum efficiency is recorded for H2 production at wavelength 420 nm.This enhanced performance is attributed to the improved Charge separation and the surface plasmon resonance effect of Au nanoparticles.Solid-state density functional theory simulations are performed to countercheck and validate our experimental data.Positive surface formation energy,high charge transfer,and strong non-bonding interaction via electrostatic forces confirm the stability of 4Au/6%WO3/CN interface.

关键词： Polymeric g-C_(3)N_(4) Plasmonic Au Charge separation Solar H_(2) production DFT calculations

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Facilely anchoring Cu_(2)O nanoparticles on mesoporous TiO_(2)nanorods for enhanced photocatalytic CO_(2)reduction through efficient charge transfer

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Chinese Chemical Letters 2022年第8期33卷 3709-3712页

作者： Ge Yang Pei Qiu Jinyan Xiong Xueteng Zhu Gang Cheng School of Chemistry and Environmental Engineering Wuhan Institute of TechnologyDonghu New&High Technology Development ZoneWuhan 430205China College of Chemistry and Chemical Engineering Wuhan Textile UniversityWuhan 430200China

Semiconductor-employed photocatalytic CO_(2) reduction has been regarded as a promising approach for environmental-friendly conversion of CO_(2) into solar fuels.Herein,TiO_(2)/Cu_(2)O composite nanorods have been successfully fabricated by a facile chemical reduction method and applied for photocatalytic CO_(2) reduction.The composition and structure characterization indicates that the Cu_(2)O nanoparticles are coupled with TiO_(2) nanorods with an intimate contact.Under light illumination,all the TiO_(2)/Cu_(2)O composite nanorods enhance the photocatalytic CO_(2)reduction.In particular,the TiO_(2)/Cu_(2)O-15%sample exhibits the highest CH_(4)yield(1.35μmol g^(-1)h^(-1)) within 4 h irradiation,and it is 3.07 and 15 times higher than that of pristine TiO_(2)nanorods and Cu_(2)O nanoparticles,respectively.The enhanced photoreduction capability of the TiO_(2)/Cu_(2)O-15%is attributed to the intimate construction of Cu_(2)O nanoparticles on TiO_(2) nanorods with formed p-n junction to accelerate the separation of photogenerated electron-hole pairs.This work provides a reference for rational design of a p-n heterojunction photocatalyst for CO_(2) photoreduction.

关键词： TiO_(2)/Cu_(2)O composite Photocatalytic CO_(2)reduction Photocatalysis Charge separation p-n Junction

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富氧空位修饰的铋氧硫晶体用于光催化二氧化碳还原转化为甲烷

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Science China Materials 2021年第9期64卷 2230-2241页

作者：姜丽莎李源吴晓勇张高科 State Key Laboratory of Silicate Materials for Architectures Hubei Key Laboratory of Mineral Resources Processing and EnvironmentWuhan University of TechnologyWuhan 430070China Shenzhen Research Institute of Wuhan University of Technology Shenzhen 518000China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450052China

制备高效光催化剂将二氧化碳还原转化为有价值的化学品,是缓解能源危机和环境污染的有效措施.本论文通过高温焙烧法,制备了富氧空位修饰的Bi_(2)O_(2)S光催化剂,并将其用于可见光驱动的CO_(2)光还原,确定了富氧空位修饰的Bi_(2)O_(2)S... 详细信息

制备高效光催化剂将二氧化碳还原转化为有价值的化学品,是缓解能源危机和环境污染的有效措施.本论文通过高温焙烧法,制备了富氧空位修饰的Bi_(2)O_(2)S光催化剂,并将其用于可见光驱动的CO_(2)光还原,确定了富氧空位修饰的Bi_(2)O_(2)S光催化剂的最佳制备条件.通过一系列实验及表征,证实了BiOS-OV中丰富氧空位的存在;结合理论计算深入分析了引入的丰富氧空位对Bi_(2)O_(2)S光催化剂的内部电子结构及光化学性能等的影响.深入研究了整个体系中光催化CO_(2)还原反应的具体步骤,旨在揭示丰富氧空位的存在引起CO_(2)光还原性能提高的根本原因.

关键词： oxygen vacancies bismuth oxysulfide Charge separation photocatalysis CO_(2)reduction

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Orthogonal carbazole-perylene bisimide pentad:a photoconversion-tunable photosensitizer with diversified excitation and excited-state relaxation pathways

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Science China Chemistry 2021年第12期64卷 2193-2202页

作者： Zhaolong Wang Yue Sun Simin Lin Gang Wang Xingmao Chang Xinyu Gou Taihong Liu Shengye Jin Gang He Yu-Chen Wei Pi-Tai Chou Yu Fang Key Laboratory of Applied Surface and Colloid Chemistry of Ministry of Education School of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an710119China College of Life Sciences Shaanxi Normal UniversityXi’an710119China State Key Laboratory of Molecular Reaction Dynamics and Collaborative Innovation Center of Chemistry for Energy Materials(iChEM) Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China Frontier Institute of Science and Technology Xi’an Jiaotong UniversityXi’an710054China Department of Chemistry Taiwan UniversityTaipei10617China

Integrating multiple photosensitive properties into an“all-in-one”photosensitizer(PS)shows great promise for the treatment of cancers owing to synergistic effect among them.However,the development of such PSs,especially those that need a single laser source,remains a challenge.Herein,we report an orchestration of electron donors and acceptors in a propeller-like pentad,PBI-4Cz,where four carbazole(Cz)units are covalently linked to the ortho-positions of the perylene bisimide(PBI)core.Strong intramolecular donor-acceptor interaction significantly quenches the luminescence and largely extends the absorption spectra to near-infrared region.Excited-state dynamics investigated via femto-and nano-second transient absorption spectroscopy revealed exclusive Charge separation of the PBI-4Cz within initial 0.5 ps when photoexcited regardless of which intermediate is involved.Energy dissipation of the resulting charge-separated state(PBI^(•−)-4Cz^(•−))is subjected to the toggle between intersystem-crossing toward excited triplet states and charge recombination toward ground states.Relative importance of the two pathways can be tuned by micro-environmental polarity,which endows PBI-4Cz remarkable performances of singlet-oxygen generation(>90.0%)in toluene and photothermal conversion(∼28.6%)in DMSO.Harnessing intrinsic photostability and excited-state processes of heavy-atom-free PBI derivatives not only holds a promise for multifunctional phototheranostics,but also provides a prototype for designing high-performance PSs with tunable photoconversion pathways.

关键词： charge recombination Charge separation perylene bisimide derivatives photosensitizers singlet oxygen generation

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Chelation-mediated in-situ formation of ultrathin cobalt(oxy)hydroxides on hematite photoanode towards enhanced photoelectrochemical water oxidation

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Journal of Energy Chemistry 2021年第5期30卷 152-161页

作者： Zhenzhen Wang Jiayue Rong Jiaqi Lv Ruifeng Chong Ling Zhang Li Wang Zhixian Chang Xiang Wang Henan Joint International Research Laboratory of Environmental Pollution Control Materials Henan Provincial Engineering Research Center of Green Anticorrosion Technology for Magnesium AlloysCollege of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004HenanChina Chemical Science Division and Center for Nanophase Materials Sciences Oak Ridge National LaboratoryOak RidgeTN 37831United States

In this work,a facile chelation-mediated route was developed to fabricate ultrathin cobalt(oxy)hydroxides(CoOOH)nanosheets on hematite photoanode(Fe_(2)O_(3)).The route contains two steps of the adsorption of[Co-EDTA]^(2-)species on Fe_(2)O_(3) nanorod array followed by the hydrolysis in alkaline solution.The resulting CoOOH/Fe_(2)O_(3) exhibits a remarkably improved photocurrent density of 2.10 mA cm^(-2) at 1.23 V vs.RHE,which is ca.2.8 times that of bare Fe_(2)O_(3).In addition,a negative shift of onset potential ca.200 mV is achieved.The structural characterizations reveal the chelate EDTA plays important roles that enhance the adsorption of Co species and the formation of contact between CoOOH and Fe_(2)O_(3).(Photo)electrochemical analysis suggests,besides providing active sites for water oxidation,CoOOH at large extent promotes the Charge separation and the charge transfer via passivating surface states and suppressing charge recombination.It also found CoOOH possesses some oxygen vacancies,which could act as trapping centers for photogenerated holes and facilitate the Charge separation.Intensity modulated photocurrent spectroscopy(IMPS)shows that,under low applied potential the water oxidation mainly occurs on CoOOH,while under high applied potential the water oxidation could occur on both CoOOH and Fe_(2)O_(3).The findings not only provide an efficient strategy for designing ultrathin(oxy)hydroxides on semiconductors for PEC applications but also put forward a new insight on the role of CoOOH during water oxidation.

关键词： Hematite Cobalt(oxy)hydroxides Photoelectrochemical water oxidation Charge separation

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