Selective Reduction of CO2 to CO by a Molecular Re(ethynyl-bpy)(CO)3Cl Catalyst and Attachment to Carbon Electrode Surfaces
Selective Reduction of CO2 to CO by a Molecular Re(ethynyl-bpy)(CO)3Cl Catalyst and Attachment to Carbon Electrode Surfaces
复制标题
Re(ethynyl-bpy)(CO)3Cl 分子催化剂将 CO2 选择性还原为 CO 并附着在碳电极表面
作者：
Almagul Zhanaidarova;Andrew L. Ostericher;Christopher J. Miller;S. C. Jones;C. Kubiak
研究了Re（乙炔基-bpy）（CO）_3Cl和Re（乙烯基-bpy）（CO）_3Cl的催化性能，并与文献报道的Re（tBu-bpy））CO）_3Cl进行了比较。Re（ethynyl-bpy）（CO）_3Cl作为分子催化剂，具有较低的过电位（η = 0.525 V）、较高的CO选择性（FE 96%）和较高的反应速率（Icat/Ip = 27）。催化剂在无水乙腈溶液中在玻碳电极表面进行电聚合，产生在CO2气氛下具有电活性的聚合物膜。在三氟乙醇（TFE）（pKa 35.4，MeCN）的存在下，这些膜表现出高效率的CO（FECO 97%）。在初步研究的基础上，这些电极显示出作为多相电催化剂的前景。为了使这些系统实用化，需要进一步优化和了解失活途径。乙炔基功能化的Re（乙炔基-bpy）（CO）3Cl催化剂也可以附着在石墨碳电极上。
The catalytic properties of Re(ethynyl-bpy)(CO)3Cl and Re(vinyl-bpy)(CO)3Cl were studied and compared with those of the previously reported Re(tBu-bpy))CO)3Cl. As a molecular catalyst, Re(ethynyl-bpy)(CO)3Cl reduces CO2 to CO with lower overpotential (η ≈ 0.525 V), higher selectivity for CO (FE 96%), and higher reaction rate (Icat/Ip = 27) compared to similar catalysts reported to date. The catalyst undergoes electropolymerization at the surface of a glassy carbon electrode in dry acetonitrile solution, creating a polymer film that is electroactive under a CO2 atmosphere. In the presence of trifluoroethanol (TFE) (pKa 35.4, MeCN) these films exhibit high efficiencies for CO (FECO 97%). On the basis of preliminary studies, these electrodes show promise as heterogeneous electrocatalysts. Further optimization and understanding of deactivation pathways will be required to make these systems practical. The ethynyl functionalized Re(ethynyl-bpy)(CO)3Cl catalyst also can be attached to graphitic carbon electrode...
影响因子：
15
作者：
Jackson, Megan N.;Oh, Seokjoon;Surendranath, Yogesh
通讯作者：
Surendranath, Yogesh