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Rational design of eco-friendly Mn-doped nonstoichiometric CuInSe/ZnSe core/shell quantum dots for boosted photoelectrochemical efficiency

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Nano Research 2022年第8期15卷 7614-7621页

作者： Rui Wang Xin Tong Zhihang Long Ali Imran Channa Hongyang Zhao Xin Li Mengke Cai Yimin You Xuping Sun Zhiming Wang Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhou 313001China Institute for Advanced Study Chengdu UniversityChengdu 610106China Department of Materials Science and Engineering Hongik UniversitySeoul 04066Republic of Korea

Colloidal core/shell quantum dots(QDs)with environment-friendly feature and controllable optoelectronic properties are promising building blocks in emerging solar *** this work,we rationally design and tailor the eco-friendly CuInSe(CISe)/ZnSe core/shell QDs by Mn doping and stoichiometric optimization(i.e.,molar ratios of Cu/In).It is demonstrated that Mn doping in In-rich CISe/ZnSe core/shell QDs can effectively engineer the charge kinetics inside the QDs,enabling efficient photogenerated electrons transfer into the shell for retarded charge *** a result,a solar-driven photoelectrochemical(PEC)device fabricated using the optimized Mn-doped In-rich CISe/ZnSe core/shell QDs(Cu/In ratio of 1/2)exhibits improved charge extraction and injection,showing a~3.5-fold higher photocurrent density than that of the pristine CISe/ZnSe core/shell QDs under 1 sun AM 1.5G *** findings indicate that transition metal doping in“green”nonstoichiometric core/shell QDs may offer a new strategy for achieving high-efficiency solar energy conversion applications.

关键词： eco-friendly colloidal quantum dot transition metal doping optoelectronic engineering photoelectrochemical cell

Promoted reverse water-gas shift activity on transition metals-incorporated iron-cerium oxide solid solution catalyst

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Progress in Natural Science:Materials International 2024年第4期34卷 676-681页

作者： Yi Xie Wenhao Qin Linyu Wang Yueren Liu Haoyang Jiang Miao Zhong College of Engineering and Applied Sciences National Laboratory of Solid State Microstructures The Frontiers Science Center for Critical Earth Material Cycling Nanjing University

Earth-abundant Fe oxide-based catalysts, renowned for their broad-spectrum light absorption, hold promise for driving the photothermal RWGS reaction—a promising strategy for converting CO2emissions into valuable carbonaceous feedstocks. However, traditional Fe oxide-based catalysts exhibit limited activity due to their constrained H2dissociation and CO2activation capabilities, especially at lower temperatures. This study introduces Co, Ni, and Cu-doped Ce0.7Fe0.3O2solid-solution catalysts. Incorporation of Fe into CeO2enhances CO2dissociation while preserving extensive light adsorption up to 2500 nm. Notably, Co doping enhances H2dissociation and promotes CO2activation. Subsequent investigations reveal that a catalyst doped with 5 mol% Co exhibits the highest photothermal catalytic activity, attaining a ～50 % CO2conversion under 300 W Xe-lamp irradiation with excellent selectivity and stability over 10 reaction cycles spanning 10 h. These results underscore the potential of designing CeO2-based solid solution catalysts with synergistic metal dopants for efficient and selective CO2conversion under moderate conditions.

关键词： Ceria Iron-based catalyst Reverse water-gas shift reaction Solid solution transition metal doping

Enhancing hydrogen evolution reaction performance of transition metal doped two-dimensional electride Ca_(2)N

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Chinese Chemical Letters 2023年第6期34卷 487-491页

作者： Baoyu Liu Ziqiang Chen Rui Xiong Xuhui Yang Yinggan Zhang Teng Xie Cuilian Wen Baisheng Sa Multiscale Computational Materials Facility and Key Laboratory of Eco-materials Advanced TechnologyCollege of Materials Science and EngineeringFuzhou UniversityFuzhou 350100China College of Environmental Science and Engineering Fujian Key Laboratory of Pollution Control&Resource ReuseFujian Normal UniversityFuzhou 350007China College of Materials Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryXiamen UniversityXiamen 361005China

Two-dimensional electride Ca_(2)N has strong electron transfer ability and low work function,which is a potential candidate for hydrogen evolution reaction(HER)*** this work,based on density functional theory calculations,we adopt two strategies to improve the HER catalytic activity of Ca_(2)N monolayer:introducing Ca or N vacancy and doping transition metal atoms(TM,refers to Ti,V,Cr,Mn,Fe,Zr,Nb,Mo,Ru,Hf,Ta and W).Interestingly,the Gibbs free energyΔG_(H*)of Ca_(2)N monolayer after introducing N vacancy is reduced to-0.146 e V,showing good HER catalytic *** is highlighted that,the HER catalytic activity of Ca_(2)N monolayer can be further enhanced with TM doping,the Gibbs free energyΔG_(H*)of single Mo and double Mn doped Ca_(2)N are predicted to be 0.119 and 0.139 e V,*** present results will provide good theoretical guidance for the HER catalysis applications of two-dimensional electride Ca_(2)N monolayer.

关键词： Two-dimensional electride Ca_(2)N Density functional theory calculations Hydrogen evolution reaction transition metal doping

doping-induced metal–N active sites and bandgap engineering in graphitic carbon nitride for enhancing photocatalytic H_(2 )evolution performance

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Chinese Journal of Catalysis 2022年第2期43卷 421-432页

作者： Xiaohui Yu Haiwei Su Jianping Zou Qinqin Liu Lele Wang Hua Tang Engineering Institute of Advanced Manufacturing and Modern Equipment Technology Jiangsu UniversityZhenjiang 212013JiangsuChina Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063JiangxiChina School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina School of Environmental Science and Engineering Qingdao UniversityQingdao 266071ShandongChina

Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subjected to atomic-level structural engineering by doping with transition metals(M=Fe,Co,or Ni),which simultaneously induced the formation of metal-N active sites in the g-C_(3)N_(4)framework and modulated the bandgap of g-C_(3)N_(4).Experiments and density functional theory calculations further verified that the as-formed metal-N bonds in M-doped g-C_(3)N_(4)acted as an"electron transfer bridge",where the migration of photo-generated electrons along the bridge enhanced the efficiency of separation of the photogenerated charges,and the optimized bandgap of g-C_(3)N_(4)afforded stronger reduction ability and wider light *** a result,doping with either Fe,Co,or Ni had a positive effect on the HER activity,where Co-doped g-C_(3)N_(4)exhibited the highest *** findings illustrate that this atomic-level structural engineering could efficiently improve the HER activity and inspire the design of powerful photocatalysts.

关键词： g-C_(3)N_(4) Photocatalytic H_(2)generation metal-N active sites transition metal doping Band gap engineering

Creation of Mo active sites on indium oxide microrods for photocatalytic amino acid production

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Science China Materials 2022年第5期65卷 1285-1293页

作者： Mang Zheng Qi Li Mingyang Liu Jianan Liu Chen Zhao Xudong Xiao Hongli Wang Jing Zhou Liping Zhang Baojiang Jiang School of Chemistry and Materials Science Heilongjiang UniversityHarbin 150080China College of Material Science and Chemical Engineering Harbin Engineering UniversityHarbin 150001China Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China

As an n-type semiconductor, In_(2)O_(3)is considered a promising photocatalyst for producing amino acids using biomass derivatives as precursors. However, similar to other intrinsic semiconductors, In_(2)O_(3)suffers from poor charge dynamics. Herein, we show the synthesis of Mo-doped In_(2)O_(3)(Mo-In_(2)O_(3)) with a porous rod-shaped structure through a onestep solvothermal reaction followed by calcination. Under visible-light irradiation, Mo-In_(2)O_(3)achieves a high conversion rate of 81% for the reaction that transforms lactic acid into alanine with a selectivity of 91%. Spectroscopic techniques and density functional theory calculations reveal that Mo doping introduces defect states slightly below the conduction band of In_(2)O_(3), which improves the separation of photogenerated electron-hole pairs. In addition, Mo atoms on the surface form extra adsorption and reaction centers that greatly enhance the reaction rate. This work provides insights into the development of transition metal-doped semiconductor photocatalysts to produce amino acids.

关键词： photocatalysis In_(2)O_(3) transition metal doping charge transfer organic synthesis