Reduced State of Iridium PCP Pincer Complexes in Electrochemical CO2 Hydrogenation

被引：20
|
作者：
Osadchuk, Irina [1 ,2 ]
Tamm, Toomas [1 ,2 ]
Ahlquist, Marten S. G. [1 ]
机构：
[1] KTH Royal Inst Technol, Sch Biotechnol, Div Theoret Chem & Biol, S-10691 Stockholm, Sweden
[2] Tallinn Univ Technol, Dept Chem, Akad Tee 15, EE-12618 Tallinn, Estonia
来源：
ACS CATALYSIS | 2016年 / 6卷 / 06期
关键词：
iridium; electrochemical reduction; hydrogenation; CO2; reduction; carbon dioxide; formate; DFT; reaction mechanism; EFFECTIVE CORE POTENTIALS; SELECTIVE ELECTROCATALYTIC REDUCTION; SOLVATION FREE-ENERGIES; CARBON-DIOXIDE; MOLECULAR CALCULATIONS; BICARBONATE REDUCTION; FORMATE; WATER; CONVERSION; IRON;
D O I：
10.1021/acscatal.6b01233
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
We present a computational study on the mechanism for electrochemical reduction of CO2 using a PCP pincer iridium(III) dihydride complex. Our results point toward a mechanism that involves an in situ-generated iridium(I) hydride as the active species for the CO2 to formate reduction. The iridium(III) path can operate in parallel but is associated with higher activation free energies in the reaction between the metal hydride and CO2, compared to the reaction at the in situ-generated iridium(I) species.
引用
收藏
页码：3834 / 3839
页数：6
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