Covalent Attachment of a Rhenium Bipyridyl CO2 Reduction Catalyst to Rutile TiO2
Covalent Attachment of a Rhenium Bipyridyl CO2 Reduction Catalyst to Rutile TiO2
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DOI：
10.1021/ja2013664
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发表时间：
2011-05-11
影响因子：
15
通讯作者：
Lian, Tianquan
中科院分区：
文献类型：
--
作者：
Anfuso, Chantelle L.;Snoeberger, Robert C., III;Lian, Tianquan
本文研究了CO_2还原电催化剂ReCO_0A（Re（CO）（3）-Cl（dcbpy）（dcbpy = 4，4 ′-二羧基-2，2 ′-联吡啶））与TiO_2金红石（001）表面的共价键合。基于和频产生（SFG）光谱和密度泛函理论（DFT）计算的分析表明，ReC 0A通过二齿或三齿连接基序中的羧酸酯基团与TiO 2结合。吸附的络合物具有dcbpy部分几乎垂直于TiO 2表面和Re暴露于溶液中的配置适合于催化。
We have characterized the covalent binding of the CO2 reduction electrocatalyst ReC0A (Re(CO)(3)-Cl(dcbpy) (dcbpy =4,4'-dicarboxy-2,2'-bipyridine)) to the TiO2 rutile (001) surface. The analysis based on sum frequency generation (SFG) spectroscopy and density functional theory (DFT) calculations indicates that ReC0A binds to TiO2 through the carboxylate groups in bidentate or tridentate linkage motifs. The adsorbed complex has the dcbpy moiety nearly perpendicular to the TiO2 surface and the Re exposed to the solution in a configuration suitable for catalysis.