ARTIFICIAL PHOTOSYNTHESIS USING PHOTOCATALYTIC MULTINUCLEAR TRANSITION METAL SIT

使用光催化多核过渡金属 SIT 进行人工光合成

• 批准号: 8362128
• 负责人: Heinz Frei
• 金额: $ 1.04万
• 依托单位: STANFORD UNIVERSITY
• 依托单位国家: 美国
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-03-01 至 2012-02-29
• 项目状态: 已结题
• 来源: https://reporter.nih.gov/project-details/8362128
• 关键词: Area; Carbon Dioxide; Catalytic Domain; Charge; Coupling; Environment; Evolution; Funding; Goals; Grant; Link; Metals; National Center for Research Resources; Optics; Oxidation-Reduction; Oxygen; Photosynthesis; Principal Investigator; Radiation; Reaction; Research; Research Infrastructure; Resources; Silicon Dioxide; Site; Source; Spectrum Analysis; Structure; Surface; Transition Elements; United States National Institutes of Health; Visible Radiation; Water; catalyst; chromophore; cost; oxidation; scaffold; structural biology

This subproject is one of many research subprojects utilizing the resources provided by a Center grant funded by NIH/NCRR. Primary support for the subproject and the subproject's principal investigator may have been provided by other sources, including other NIH sources. The Total Cost listed for the subproject likely represents the estimated amount of Center infrastructure utilized by the subproject, not direct funding provided by the NCRR grant to the subproject or subproject staff. Visible light-absorbing polynuclear charge-transfer sites anchored on the pore surface of high surface area mesoporous silica afford splitting of carbon dioxide to CO. Polynuclear water oxidation catalysts can be covalently linked to metal centers embedded in the silica pore surface for oxygen evolution under visible light. Evidence for covalent anchoring on the silica surface and connection of the metal centers through an O bridge was obtained by FT-infrared, FT-Raman and optical spectroscopy. In order to reach our long term goal of coupling the photocatalytic components of the half reactions to build integrated units in these nanoporous scaffolds that reduced CO2 by H2O under visible light, a more detailed structural understanding of the redox sites is essential. Therefore, XAS studies are proposed with the goal of elucidating the coordination environment of the metal centers of the binuclear charge-transfer chromophores, and the precise structure of the linkage between the donor metal center and the catalytic core of the water oxidation catalyst.

该子项目是利用资源的众多研究子项目之一 由 NIH/NCRR 资助的中心拨款提供。子项目的主要支持 并且子项目的主要研究者可能是由其他来源提供的， 包括其他 NIH 来源。 子项目可能列出的总成本 代表子项目使用的中心基础设施的估计数量， NCRR 赠款不直接向子项目或子项目工作人员提供资金。 固定在高表面积介孔二氧化硅的孔表面上的可见光吸收多核电荷转移位点可将二氧化碳分解为 CO。多核水氧化催化剂可以与嵌入二氧化硅孔表面的金属中心共价连接，以便在可见光下析出氧气。通过 FT-红外、FT-拉曼和光谱获得了二氧化硅表面上的共价锚定以及金属中心通过 O 桥连接的证据。为了实现我们的长期目标，即耦合半反应的光催化成分，在这些纳米多孔支架中构建集成单元，在可见光下通过 H2O 还原 CO2，对氧化还原位点进行更详细的结构了解至关重要。因此，XAS研究的目的是阐明双核电荷转移发色团金属中心的配位环境，以及供体金属中心与水氧化催化剂催化核心之间连接的精确结构。