Kumar Amit, Janes Trevor, Espinosa-Jalapa Noel Angel, Milstein David
Department of Organic Chemistry, Weizmann Institute of Science, Rehovot, 76100, Israel.
Current address: Institut für Anorganische Chemie, Universität Regensburg, 93053, Regensburg, Germany.
Angew Chem Int Ed Engl. 2018 Sep 10;57(37):12076-12080. doi: 10.1002/anie.201806289. Epub 2018 Aug 7.
The first example of a homogeneous catalyst based on an earth-abundant metal for the hydrogenation of organic carbonates to methanol and alcohols is reported. Based on the mechanistic investigation, which indicates metal-ligand cooperation between the manganese center and the N-H group of the pincer ligand, we propose that the hydrogenation of organic carbonates to methanol occurs via formate and aldehyde intermediates. The reaction offers an indirect route for the conversion of CO to methanol, which coupled with the use of an earth abundant catalyst, makes the overall process environmentally benign and sustainable.
报道了首例基于储量丰富的金属的均相催化剂,用于将有机碳酸酯氢化为甲醇和醇类。基于机理研究表明锰中心与钳形配体的N-H基团之间存在金属-配体协同作用,我们提出有机碳酸酯氢化为甲醇是通过甲酸盐和醛中间体进行的。该反应为将CO转化为甲醇提供了一条间接途径,再结合使用储量丰富的催化剂,使得整个过程对环境友好且可持续。