期刊
ORGANOMETALLICS
卷 38, 期 15, 页码 3084-3091出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.organomet.9b00413
关键词
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资金
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Catalysis Science Program [DE-SC0018222]
- U.S. Department of Energy (DOE) [DE-SC0018222] Funding Source: U.S. Department of Energy (DOE)
Methanol is a crucial precursor for the preparation of many high-value commercial chemicals and synthesizing it from an inexpensive and renewable carbon source such as carbon dioxide (CO2) could have significant benefits. Herein, a homogeneous iron(II) pincer complex for the catalytic generation of methanol from CO2 and H-2 via a two-step process is described. The CO2 reduction process occurs through initial coupling with H-2 and an amine to give a formamide. Subsequently, the formamide undergoes catalytic deaminative hydrogenation to afford methanol and regenerate the amine. A net turnover number of 590 is obtained for CO2 and H-2 to methanol using this method. The primary obstacle to a single-batch catalytic process is CO2 poisoning of the catalyst in the formamide hydrogenation step, and mechanistic investigations suggest that this CO2 inhibition results from the formation of a stable iron(II) formate complex.
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