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Photocatalysis in solar fuel production

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National Science Review 2015年第2期2卷 145-147页

作者： hongxian han Can Li State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences and Dalian National Laboratory for Clean Energy

With the increasing concerns on energy and environmental problems caused by the combustion of fossil fuels,solar energy becomes vitally important because it is the only viable renewable energy source that can replace ... 详细信息

关键词： PSP

EPR study of charge separation associated states and reversibility of surface bound superoxide radicals in SrTiO_(3) photocatalyst

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Journal of Energy Chemistry 2022年第7期31卷 388-393,I0011页

作者： Xianwen Zhang Zheng Li Bin Zeng Can Li hongxian han State Key Laboratory of Catalysis and Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Understanding the processes of charge generation, transfer and capture is important for the design and synthesis of efficient photocatalysts. In this work, light-induced charge separation and effect of O_(2) on electron transfer processes in SrTiO_(3) were investigated by electron paramagnetic resonance(EPR). It was found that photoinduced electron transfer from O_(2)- to Ti^(4+) produced Ti^(3+) and O- redox radical pairs under vacuum condition. Under oxygen atmosphere, however, surface bound superoxide radicals O_(2)-were formed by electron reduction of adsorbed oxygen at initial photoirradiation stage, and quenched by the reverse electron transfer to Ti^(4+) upon further photoirradiation. Formation of long-lived charge separation associated [Ti^(3+)---O-] species and the reversibility of surface bound superoxide radicals mediating the processes of photogenerated electrons may be accountable for the high activity of SrTiO_(3) in photocatalytic water splitting reaction.

关键词： Photocatalyst Electron paramagnetic resonance Charge separation Superoxide radicals

Preface to the Special Issue of Photocatalysis for Solar Fuels

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Chinese Journal of Catalysis 2018年第3期39卷 367-368页

作者：韩洪宪刘岗 State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences School of Future Technology University of Chinese Academy of Sciences Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of Sciences College of Materials Science and Engineering University of Science and Technology of China

As natural photosynthesis does, direct conversion of solar energy into the storable form of chemical energy is an intriguing technology for solar energy utilization. Due to increasing concerns of energy and environmental problems caused by the consumption of fossil fuels, production of chemical solar fuels (such as hydrogen, methanol or methane,etc) by artificial photosynthesis, namely photocatalytic splitting of water or reduction of CO2, has been a hot research topic in recent years.

关键词： As natural photosynthesis does, direct conversion of solar energy

A Novel Sr_2CuInO_3S p-type semiconductor photocatalyst for hydrogen production under visible light irradiation

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Journal of Energy Chemistry 2014年第4期23卷 420-426页

作者： Yushuai Jia Jingxiu Yang Dan Zhao hongxian han Can Li State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian National Laboratory for Clean Energy

A novel Sr2CulnO3S oxysulfide p-type semiconductor photocatalyst has been prepared by solid state reaction method and it exhibits intriguing visible light absorption properties with a bandgap of 2.3 eV. The p-type semiconductor character of the synthesized Sr2CuInO3 S was confirmed by Hall efficient measurement and Mott-Schottky plot analysis. First-principles density functional theory calculations （DFT） and electrochem ical measurements were performed to elucidate the electronic structure and the energy band locations. It was found that the as-synthesized Sr2CuInO3S photocatalyst has appreciate conduction and valence band positions for hydrogen and oxygen evolution, respectively. Photocat alytic hydrogen production experiments under a visible light irradiation （A〉420 nm） were carried out by loading different metal and metal-like cocatalysts on Sr2CuInO3S and Rh was found to be the best one among the tested ones.

关键词： hydrogen production photocatalyst p-type semiconductor Sr2CuIn03S oxysulfide visible light cocatalyst

La and CrCo-doped SrTiO_3 as an H_2 evolution photocatalyst for construction of a Z-scheme overall water splitting system

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Chinese Journal of Catalysis 2018年第3期39卷 421-430页

作者： Yushuai Jia Dan Zhao Mingrun Li hongxian han Can Li State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Liaoning China College of Chemistry and Chemical Engineering Jiangxi Normal University Nanchang 330022 Jiangxi China

The photocatalytic activity of a semiconductor‐based photocatalyst largely depends on the semiconductor’s intrinsic crystal and electronic *** have prepared two types of La and Cr co‐doped SrTiO3photocatalysts(SrTiO3(La,Cr))using the polymerized complex method(PCM)and sol‐gel hydrothermal method(SHM).Under?>420‐nm visible light irradiation,only the Pt‐loaded SrTiO3(La,Cr)prepared by the SHM showed efficient photocatalytic activities for both H2evolution in the presence of an I?sacrificial reagent and for Z‐scheme overall water splitting when it was coupled with the Pt‐loaded WO3in the presence of I?and IO3?as the shuttle redox *** superior photocatalytic activity of SrTiO3(La,Cr)prepared by the SHM has been ascribed to its more negative conduction‐band position,higher carrier concentration,and higher carrier mobility,demonstrating that the design and synthesis of an H2‐evolution photocatalyst with appropriate electronic properties is crucial for achieving Z‐scheme overall water splitting.

关键词： Strontium titanate Photocatalysis Water splitting Z‐scheme Hydrogen evolution

p-Type CaFe_2O_4 semiconductor nanorods controllably synthesized by molten salt method

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Journal of Energy Chemistry 2016年第3期25卷 381-386页

作者： Xin Liu Junzhe Jiang Yushuai Jia Ailing Jin Xiangshu Chen Fei Zhang hongxian han Jiangxi Inorganic Membrane Materials Engineering Research Centre College of Chemistry and Chemical Engineering Jiangxi Normal University State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian National Laboratory for Clean Energy

Pure phase, regular shape and well crystallized nanorods of p-type semiconductor CaFeOhave been fabricated for the first time by a facile molten salt assisted method, as confirmed by XRD, TEM, SEM and HRTEM. UV-vis diffuse reflectance spectra and Mott–Schottky plots show that the band structure of the CaFeOnanorods is narrower than that of the CaFeOnanoparticles synthesized by conventional method. The enhancement of the visible-light absorption is due to narrowness of the band gap in CaFeOnanorods. The appropriate ratio between the molten salt and the CaFeOprecursors plays an important role in inhibiting the growth of the crystals along the(201) plane to give the desired nanorod morphology. This work not only demonstrates that highly pure p-type CaFeOsemiconductor with tunable band structure and morphology could be obtained using the molten salt strategy, but also affirms that the bandgap of a semiconductor may be tunable by monitoring the growth of a particular crystal ***, the facile eutectic molten salt method developed in this work may be further extended to fabricate some other semiconductor nanomaterials with a diversity of morphologies.

关键词： p-Type semiconductor CaFe_2O_4 nanorods Molten salt Crystal plane Visible-light absorption

Intrinsic photocatalytic water oxidation activity of Mn-doped ferroelectric BiFeO3

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Chinese Journal of Catalysis 2021年第6期42卷 945-952页

作者： Jafar Hussain Shah Anum Shahid Malik Ahmed Mahmoud Idris Saadia Rasheed hongxian han Can Li State Key Laboratory of Catalysis&Division of Solar Energy Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

The development of stable and efficient visible light-absorbing oxide-based semiconductor photocatalysts is a desirable task for solar water splitting ***,we proposed that the low photocurrent density in film-based BiFeO_(3)(BFO)is due to charge recombination at the interface of the domain walls,which could be largely reduced in particulate photocatalyst *** demonstrate this hypothesis,in this work we synthesized particulate BFO and Mn-doped BiFeO_(3)(Mn-BFO)by the sol-gel *** water oxidation tests showed that pure BFO had an intrinsic photocatalytic oxygen evolution reaction(OER)activity of 70μmol h^(-1) g^(-1),while BFO-2,with an optimum amount of Mn doping(0.05%),showed an OER activity of 255μmol h^(-1) g^(-1) under visible light(λ≥420 nm)*** bandgap of Mn-doped BFO could be reduced from 2.1 to 1.36 eV by varying the amount of Mn *** functional theory(DFT)calculations suggested that surface Fe(rather than Mn)species serve as the active sites for water oxidation,because the overpotential for water oxidation on Fe species after Mn doping is 0.51 V,which is the lowest value measured for the different Fe and Mn species examined in this *** improved photocatalytic water oxidation activity of Mn-BFO is ascribed to the synergistic effect of the bandgap narrowing,which increases the absorption of visible light,reduces the activation energy of water oxidation,and inhibits the recombination of photogenerated *** work demonstrates that Mn doping is an effective strategy to enhance the intrinsic photocatalytic water oxidation activity of particulate ferroelectric BFO photocatalysts.

关键词： Photocatalytic water oxidation Bandgap engineering Bismuth ferrite Ferroelectric materials Cation doping

Water oxidation sites located at the interface of Pt/SrTiO_(3) for photocatalytic overall water splitting

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Chinese Journal of Catalysis 2022年第8期43卷 2223-2230页

作者： Xianwen Zhang Zheng Li Taifeng Liu Mingrun Li Chaobin Zeng Hiroaki Matsumoto hongxian han State Key Laboratory of Catalysis and Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China National&Local Joint Engineering Research Center for Applied Technology of Hybrid Nanomaterials Henan UniversityKaifeng 475004HenanChina Hitachi High-Tech(Shanghai)Co. Ltd.Shanghai 201203China

When a proton reduction cocatalyst is loaded on an n-type semiconductor for photocatalytic overall water splitting(POWS),the location of water oxidation sites is generally considered at the surface of the semiconductor due to upward band-bending of n-type semiconductor which may ease the transfer of the photogenerated holes to the ***,this is not the case for Pt/SrTiO_(3),a model semiconductor based photocatalyst for *** was found that the photogenerated holes are more readily accumulated at the interface between Pt cocatalyst and SrTiO_(3) photocatalyst as probed by photo-oxidative deposition of PbO_(2),indicating that the water oxidation sites are located at the interface between Pt and SrTiO_(3).Electron paramagnetic resonance and scanning transmission electron microscope studies suggest that the interfacial oxygen atoms between Pt and SrTiO_(3) in Pt/SrTiO_(3) after POWS are more readily lost to form oxygen vacancies upon vacuum heat treatment,regardless of Pt loading by photodeposition or impregnation methods,which may serve as additional support for the location of the active sites for water oxidation at the *** functional theory calculations also suggest that the oxygen evolution reaction more readily occurs at the interfacial sites with the lowest *** experimental and theoretical studies reveal that the more active sites for water oxidation are located at the interface between Pt and SrTiO_(3),rather than on the surface of SrTiO_(3).Hence,the tailor design and control of the interfacial properties are extremely important for the achievement or improvement of the POWS on cocatalyst loaded semiconductor photocatalyst.

关键词： Photocatalytic overall water splitting Active site Oxygen vacancy Interface Cocatalyst

北京森林类型生态系统服务空间异质性及其影响因素分析

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北京师范大学学报（自然科学版） 2024年第3期60卷 350-357页

作者：卢奕妃李鑫豪赵洪贤韩聪刘新月毛军北京林业大学水土保持学院林木资源高效生产全国重点实验室北京

量化评价生态系统服务是合理开发森林生态资源、实现其可持续发展的重要前提.本研究以北京市不同的森林类型(针叶林、阔叶林和针阔混交林)为研究对象,定量分析其生态系统服务及其权衡关系,并利用地理探测器分析其空间异质性的主要驱动因... 详细信息

量化评价生态系统服务是合理开发森林生态资源、实现其可持续发展的重要前提.本研究以北京市不同的森林类型(针叶林、阔叶林和针阔混交林)为研究对象,定量分析其生态系统服务及其权衡关系,并利用地理探测器分析其空间异质性的主要驱动因子.结果表明:1)针叶林净初级生产力(NPP)(324.08 g·m^(-2)·a^(-1))大于阔叶林(303.33g·m^(-2)·a^(-1))和针阔混交林(291.74 g·m^(-2)·a^(-1)),环境改善服务从大到小依次为针叶林(251.91 kg·a^(-1))、混交林(215.39kg·a^(-1))、阔叶林(155.36 kg·a^(-1));阔叶林产水服务和水土保持服务较高.2)各项生态系统服务空间异质性的主要驱动因子在不同森林类型中没有明显的差别,均为气候因子;产水量和环境改善的主要驱动因子为气温和降水;NPP的主要驱动因子为降水、气温和辐射.3)产水服务与NPP和水土保持之间存在协同关系,即产水服务越大时,NPP和水土保持服务也具有较大的值.4)交互探测表明,多数因子如高程与气候因子交互后,对各项生态系统服务的空间异质性的解释力度加强.因此,在以某项生态服务功能为目的进行造林时,应注重灌溉、保墒及保温等抚育措施,并综合考虑地形因子的影响.在分析人工林生态系统服务功能时还应充分考虑不同影响因子的交互作用.

关键词：生态系统服务功能森林类型空间异质性