太阳燃料金属/C3N4表面等离子体复合光催化材料的制备和性能

Graphitic carbon nitride (g-C3N4)and plasmonic photocatalysts have been attracting great interest in recent years. However, the research on solar-to-fuels conversion using photocatalysts constructed by the new developed visible-light semiconductor g-C3N4 and plasmonic metals with strong surface plasmon resonance (SPR) effect is just at the initial stage. This project is an innovative study on the design and fabrication of hybrid photocatalysts based on the combination of g-C3N4 and plasmonic metals (Au and Ag), and their application for efficient visible-light photocatalytic hydrogen production from water reduction, as well as the CO2 reduction to produce hydrocarbon fuels. In this project, the controlled preparation of plasmonic metal/g-C3N4 hybrid photocatalysts will be achieved by tuning the morphology, size, and composition of the metals and g-C3N4. The photocatalytic mechanisms will be explored in terms of the coupling action of strong SPR effect from the metals and the visible-light response from the semiconductor g-C3N4. The inherent relationship between the composition, structure, metal loading amount of the metal/g-C3N4 hybrid photocatalysts, and the photocatalytic properties for hydrogen production and CO2 reduction will be clarified. Carrying out this project will provide both practical and theoretical guidance for the development of highly stable and efficient visible-light photocatalysts for solar-to-fuels conversion.

新型可见光半导体g-C3N4和表面等离子体光催化材料近年来受到广泛的关注，但将这两者结合用于制备太阳燃料的研究却很少见。本项目提出设计和制备基于超薄g-C3N4和具有强表面等离子体共振效应的金属（Au和Ag）的复合光催化材料，并将其应用于光催化分解水产氢和二氧化碳加氢还原制备碳氢化合物的反应当中。通过调控金属和g-C3N4的形貌、尺寸和组分等方法探索金属/g-C3N4表面等离子体光催化材料的可控制备，研究所制备材料的可见光光催化分解水产氢性能，并进一步研究其用于温室气体二氧化碳可见光光催化加氢生产甲烷甲醇等碳氢燃料的性能，探讨表面等离子体共振效应和g-C3N4可见光吸收耦合作用下的光催化机理，揭示金属/g-C3N4复合材料的组分、结构和金属负载量与光催化产氢以及二氧化碳加氢还原性能之间的内在联系，为发展高可见光利用率、高活性和高稳定性的太阳燃料光催化材料提供实验依据和理论指导。

项目执行期间通过调控金属和g-C3N4的形貌、尺寸和组分等方法探索了金属/g-C3N4表面等离子体光催化材料的可控制备，研究了所制备材料的可见光光催化分解水产氢性能，并进一步研究了其用于温室气体二氧化碳可见光光催化加氢生产甲烷甲醇等碳氢燃料的性能，探讨了表面等离子体共振效应和g-C3N4可见光吸收耦合作用下的光催化机理，揭示了金属/g-C3N4复合材料的组分、结构和金属负载量与光催化产氢以及二氧化碳加氢还原性能之间的内在联系。多篇研究论文发表在多种国内外权威刊物上，如：Advanced Materials、Advanced Functional Materials、Journal of Photochemistry and Photobiology C: Photochemistry Reviews、Applied Catalysis B: Environmental、Journal of Materials Chemistry A、Journal of Catalysis、Journal of Power Sources 等，发表SCI 收录论文17篇，其中ESI高被引论文5篇，发表论文被SCI引文1700余次。申请了国家发明专利4项。项目执行期间共毕业了6位硕士研究生，另有7位研究生在读。建立了较为广泛的国际学术交流与合作关系。项目负责人曹少文2018年入选科睿唯安“全球高被引科学家”榜单；2017年获得湖北省青年杰出人才基金资助；2016年入选武汉理工大学15551人才工程；2014年入选湖北省“楚天学者计划”；项目期间被聘为国际期刊《Scientific Reports》编委和国内期刊《Chinese Journal of Catalysis》青年编委。