Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.
Yaqiang WuJianuo LiWei-Kean ChongZhenhua PanQian Wang
β-Ga_(2)O_(3)以其较高的导带底(Conduction Band Minimum,CBM)和较低的价带顶(Valence Band Maximum,VBM),赋予其光生电子和空穴较强的还原与氧化能力,但其宽禁带和高载流子复合率限制了在光催化中的应用.金属离子掺杂被认为是提升光催化性能的有效途径.本文基于第一性原理系统研究了Sr、Ba、V、Nb、Ta等二十种元素掺杂对β-Ga_(2)O_(3)光催化性能的影响,研究发现:Sr、Nb、Ta、Mn、Fe、Zn、Hg七种元素掺杂β-Ga_(2)O_(3)后,材料除能保持合适的带边位置外,还具有更高的电子空穴分离效率以及更低的形成能,表明这些元素的引入可有效提升β-Ga_(2)O_(3)光催化效率;Nb、Ta掺杂可显著增强材料在红外光区的吸收,Mn、Fe掺杂则显著提升材料在紫外和可见光区的吸收能力,其中,Nb在0.5 eV处光吸收系数高达1.38×10^(5)cm^(−1),Mn、Fe掺杂在3 eV处光吸收系数可达1×10^(5)cm^(−1),在不同波段均呈现出良好的光吸收能力.此外,Hg掺杂表现出跨红外至深紫外的宽波段增强效果,Hg掺杂后,电子空穴相对有效质量高达109,说明Hg掺杂显著提升载流子分离能力,同时由于其在宽波段显著增强的光吸收效果,因此,Hg可作为β-Ga_(2)O_(3)在光催化制氢中理想的金属掺杂元素,以上研究结果为β-Ga_(2)O_(3)光催化分解水制氢研究提供了价值参考.
Photocatalytic water splitting using natural solar light is considered as a sustainable approach to generate H_(2) and O_(2).While H_(2) has high market value,the by-product of water splitting,oxygen,is less valuable.To make H_(2) produced by means of photocatalysis more economically competitive to that generated from methane,its generation is studied together with synthesis of organic compounds that have higher market value.This review summarizes and analyzes critically dehydrogenation reactions that were developed since 1980s.Photocatalytic dehydrogenation reactions are classified and the results are collected in the online database.Performance of homogeneous and heterogenous photocatalysts in dehydrogenation reactions,such as yield rates of organic products on analytical and preparative scales,and quantum efficiencies are compared.Current limitations of the existing methods and photocatalytic systems are identified and directions for the future developments are outlined.
