Hydrogenation of CO2 to Formate with H2: Transition Metal Free Catalyst Based on a Lewis Pair

被引：70
|
作者：
Zhao, Tianxiang [1 ]
Hu, Xingbang [1 ]
Wu, Youting [1 ]
Zhang, Zhibing [1 ]
机构：
[1] Nanjing Univ, Sch Chem & Chem Engn, Separat Engn Res Ctr, Nanjing 210093, Jiangsu, Peoples R China
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 03期
基金：
中国国家自然科学基金;
关键词：
carbon dioxide; formate; homogeneous catalysis; hydrogenation; Lewis pair; SMALL-MOLECULE ACTIVATION; CARBON-DIOXIDE; FORMIC-ACID; ENANTIOSELECTIVE HYDROGENATION; DIHYDROGEN ACTIVATION; NITROGEN MONOXIDE; METHANOL; REDUCTION; REACTIVITY; COMPLEXES;
D O I：
10.1002/anie.201809634
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Hydrogenation of CO2 to formate with H-2 in the absence of transition metal is a long-standing challenge in catalysis. The reactions between tris(pentafluorophenyl)borane (BCF) and K2CO3 (or KHCO3) are found to form a Lewis pair (K-2[(BCF)(2)-CO3]) which can react with both H-2 and CO2 to produce formate. Based on these stoichiometric reactions, the first catalytic hydrogenation process of CO2 to formate using transition metal free catalyst (BCF/M2CO3, M=Na, K, and Cs) is reported. The highest TON value of this catalytic process is up to 3941. Further research revealed the reaction mechanism in which the Lewis pair enables the splitting of H-2 and the insertion of CO2 into the B-H bond.
引用
收藏
页码：722 / 726
页数：5
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