Covalent attachment of a molecular CO2-reduction photocatalyst to mesoporous silica

Covalent attachment of a molecular CO2-reduction photocatalyst to mesoporous silica
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DOI:
10.1016/j.molcata.2012.06.011
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发表时间:
2012-11-01
影响因子:
--
通讯作者:
Li, Gonghu
Li, Gonghu
中科院分区:
化学2区
文献类型:
--
作者:
Dubois, Kevin D.;He, He;Li, Gonghu

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以介孔氧化硅为载体,通过共价结合和物理吸附的方法,成功地将分子式CO 2还原光催化剂Re(bpy)(CO)(3)Cl固定在介孔氧化硅上。共价连接的Re(I)配合物在光化学条件下表现出优异的稳定性,并且在太阳能CO2还原中比其均相对应物具有更高的活性。相反,物理吸附的Re(I)络合物表现出较差的光化学稳定性和活性。此外,共价连接的Re(I)光催化剂具有增强的吸收在可见光区由于衍生化的bpy配体与酰胺基团。我们的研究表明,通过简单的有机键的共价连接是一个很有前途的策略,将分子CO2还原光催化剂的固态表面。由爱思唯尔公司出版
A molecular CO2-reduction photocatalyst, Re(bpy)(CO)(3)Cl where bpy =2,2'-bipyridine, was successfully immobilized on mesoporous silica through covalent attachment and physical adsorption. The covalently attached Re(I) complex demonstrated excellent stability under photochemical conditions and higher activity than its homogeneous counterpart in solar CO2 reduction. In contrast, the physically adsorbed Re(I) complex showed poor photochemical stability and activity. Furthermore, the covalently attached Re(I) photocatalyst possess enhanced absorption in the visible-light region due to derivatization of the bpy ligand with amido groups. Our study suggests that covalent attachment through simple organic linkages is a promising strategy to immobilize molecular CO2-reduction photocatalysts on solid-state surfaces. Published by Elsevier B.V.