Catalytic Homogeneous Hydrogenation of CO to Methanol via Formamide
Catalytic Homogeneous Hydrogenation of CO to Methanol via Formamide
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DOI：
10.1021/jacs.9b06586
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发表时间：
2019-08-14
影响因子：
15
通讯作者：
Prakash, G. K. Surya
中科院分区：
文献类型：
--
作者：
Kar, Sayan;Goeppert, Alain;Prakash, G. K. Surya
介绍了一种新型的胺辅助CO低温均相加氢制甲醇的反应路线。反应通过形成甲酰胺中间体进行。第一胺羰基化部分由K3 PO 4催化。随后，在市售钌钳形络合物作为催化剂的存在下，将甲酰胺原位氢化成甲醇。在优化的反应条件下，CO（高达10巴）直接转化为甲醇，在H-2（70巴）和二乙烯三胺的存在下，高产率和选择性。使用催化剂Ru-Macho-BH实现了539的最大TON。在低反应温度（145摄氏度）下生产甲醇所获得的高产率、选择性和TON可能使该工艺成为传统高温多相催化的有吸引力的替代方案。
A novel amine-assisted route for low temperature homogeneous hydrogenation of CO to methanol is described. The reaction proceeds through the formation of formamide intermediates. The first amine carbonylation part is catalyzed by K3PO4. Subsequently, the formamides are hydrogenated in situ to methanol in the presence of a commercially available ruthenium pincer complex as a catalyst. Under optimized reaction conditions, CO (up to 10 bar) was directly converted to methanol in high yield and selectivity in the presence of H-2 (70 bar) and diethylenetriamine. A maximum TON of 539 was achieved using the catalyst Ru-Macho-BH. The high yield, selectivity, and TONs obtained for methanol production at low reaction temperature (145 degrees C) could make this process an attractive alternative over the traditional high temperature heterogeneous catalysis.