Hydrogenation of CO2, Hydrogenocarbonate, and Carbonate to Formate in Water using Phosphine Free Bifunctional Iron Complexes

被引:63
作者
Coufourier, Sebastien [2 ]
Gaillard, Quentin Gaignard [2 ]
Lohier, Jean-Francois [2 ]
Poater, Albert [1 ]
Gaillard, Sylvain [2 ]
Renaud, Jean-Luc [2 ]
机构
[1] Univ Girona, IQCC, Dept Quim, Girona 17003, Spain
[2] Normandie Univ, CNRS, UNICAEN, LCMT,ENSICAEN, F-14050 Caen, France
关键词
iron complexes; hydrogenation; carbon dioxide; carbonic derivatives; water-soluble complexes; catalysis; LOW-PRESSURE HYDROGENATION; FORMIC-ACID; CATALYZED HYDROGENATION; REVERSIBLE HYDROGENATION; PINCER COMPLEXES; DIOXIDE; REDUCTION; BICARBONATE; REACTIVITY; LIGAND;
D O I
10.1021/acscatal.9b04340
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
The development of efficient and low-cost catalytic systems is important for the replacement of the robust noble metal complexes. A highly efficient, stable, phosphine-free, and easy-to-synthesize iron catalyst system for the reduction of CO2, hydro-genocarbonate, and carbonate in pure water is reported. In the presence of the bifunctional cyclopentadienone iron tricarbonyl Fe4a-d, the hydrogenation of carbonic derivatives proceeds in good yields with good catalyst productivity. Turnover numbers (TON) of up to 3343, 4234, and 40 for the hydrogenation of CO2, hydrogenocarbonate, and carbonate, respectively, to formate in pure water were achieved. For the CO2 hydrogenation, a base was required, and triethanolamine emerged as the best one. DFT calculations rationalized the mechanism as well as the better performance of triethanolamine as a base.
引用
收藏
页码:2108 / 2116
页数:17
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