ARTIFICIAL PHOTOSYNTHESIS USING PHOTOCATALYTIC MULTINUCLEAR TRANSITION METAL SIT

这个子项目是许多研究子项目中利用 资源由NIH/NCRR资助的中心拨款提供。子项目和 调查员(PI)可能从NIH的另一个来源获得了主要资金， 并因此可以在其他清晰的条目中表示。列出的机构是 该中心不一定是调查人员的机构。 高比表面积介孔二氧化硅的孔表面具有可见光吸收的多核电荷转移中心，可将二氧化碳分解为CO。多核水氧化催化剂可以共价连接到镶嵌在二氧化硅孔表面的金属中心上，在可见光下析氧。通过红外光谱、拉曼光谱和光谱分析，证实了共价锚定在二氧化硅表面和金属中心通过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成分，在这些在可见光下通过H2O还原二氧化碳的纳米多孔支架中建立集成单元，对氧化还原中心的结构有更详细的了解是必不可少的。因此，提出了XAS研究，目的是阐明双核电荷转移发色团金属中心的配位环境，以及给体金属中心与水氧化催化剂催化核心之间的精确结构。

This subproject is one of many research subprojects utilizing the resources provided by a Center grant funded by NIH/NCRR. The subproject and investigator (PI) may have received primary funding from another NIH source, and thus could be represented in other CRISP entries. The institution listed is for the Center, which is not necessarily the institution for the investigator. 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.