Hydrogenation of CO2, Hydrogenocarbonate, and Carbonate to Formate in Water using Phosphine Free Bifunctional Iron Complexes
Hydrogenation of CO2, Hydrogenocarbonate, and Carbonate to Formate in Water using Phosphine Free Bifunctional Iron Complexes
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DOI：
10.1021/acscatal.9b04340
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发表时间：
2020-02-07
期刊：
影响因子：
12.9
通讯作者：
Renaud, Jean-Luc
中科院分区：
文献类型：
--
作者：
Coufourier, Sebastien;Gaillard, Quentin Gaignard;Renaud, Jean-Luc
开发高效、低成本的催化体系对于取代传统的贵金属络合物具有重要意义。报道了一种高效、稳定、无膦、易于合成的铁催化剂体系，用于纯水中CO2、碳酸氢盐和碳酸盐的还原。在双官能环烯酮三羰基铁Fe 4a-d的存在下，碳衍生物的氢化以良好的产率和良好的催化剂生产率进行。转换数（吨）高达3343，4234，和40的氢化CO2，碳酸氢盐，碳酸盐，分别在纯水中甲酸盐实现。对于CO2加氢，需要碱，三乙醇胺是最好的碱。DFT计算合理化的机制，以及更好的性能三乙醇胺作为基地。
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.