ARTIFICIAL PHOTOSYNTHESIS USING PHOTOCATALYTIC MULTINUCLEAR TRANSITION METAL SIT

这个子项目是许多利用资源的研究子项目之一 由NIH/NCRR资助的中心拨款提供。子项目的主要支持 而子项目的主要调查员可能是由其他来源提供的， 包括其它NIH来源。 列出的子项目总成本可能 代表子项目使用的中心基础设施的估计数量， 而不是由NCRR赠款提供给子项目或子项目工作人员的直接资金。 可见光吸收的多核电荷转移网站锚定在高表面积的介孔二氧化硅的孔表面提供分裂的二氧化碳CO。多核水氧化催化剂可以共价连接到嵌入在二氧化硅孔表面的金属中心，在可见光下的氧析出。通过FT-红外光谱、FT-拉曼光谱和光学光谱得到了二氧化硅表面上共价锚定和金属中心通过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组分，以在这些纳米多孔支架中构建在可见光下通过H2O还原CO2的集成单元，对氧化还原位点的更详细的结构理解是必不可少的。因此，提出了XAS研究的目的是阐明双核电荷转移发色团的金属中心的配位环境，以及供体金属中心和水氧化催化剂的催化核心之间的连接的精确结构。

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.