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钴催化剂上CO选择性加氢制乙醇

Selective Hydrogenation of CO to Ethanol over Cobalt Catalysts.

作者信息

Wang Lingxiang, Wang Liang, Zhang Jian, Liu Xiaolong, Wang Hai, Zhang Wei, Yang Qi, Ma Jingyuan, Dong Xue, Yoo Seung Jo, Kim Jin-Gyu, Meng Xiangju, Xiao Feng-Shou

机构信息

Department of Chemistry, Zhejiang University, Hangzhou, 310028, China.

Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.

出版信息

Angew Chem Int Ed Engl. 2018 May 22;57(21):6104-6108. doi: 10.1002/anie.201800729. Epub 2018 Apr 25.

DOI:10.1002/anie.201800729
PMID:29660228
Abstract

Methods for the hydrogenation of CO into valuable chemicals are in great demand but their development is still challenging. Herein, we report the selective hydrogenation of CO into ethanol over non-noble cobalt catalysts (CoAlO ), presenting a significant advance for the conversion of CO into ethanol as the major product. By adjusting the composition of the catalysts through the use of different prereduction temperatures, the efficiency of CO to ethanol hydrogenation was optimized; the catalyst reduced at 600 ° gave an ethanol selectivity of 92.1 % at 140 °C with an ethanol time yield of 0.444 mmol g  h . Operando FT-IR spectroscopy revealed that the high ethanol selectivity over the CoAlO catalyst might be due to the formation of acetate from formate by insertion of *CH , a key intermediate in the production of ethanol by CO hydrogenation.

摘要

将一氧化碳(CO)加氢转化为有价值化学品的方法需求巨大,但其开发仍具有挑战性。在此,我们报道了在非贵金属钴催化剂(CoAlO)上CO选择性加氢制乙醇的方法,这是将CO转化为主要产物乙醇方面的一项重大进展。通过使用不同的预还原温度来调整催化剂的组成,优化了CO加氢制乙醇的效率;在600°C下还原的催化剂在140°C时乙醇选择性为92.1%,乙醇时空产率为0.444 mmol g⁻¹ h⁻¹。原位傅里叶变换红外光谱表明,CoAlO催化剂上高乙醇选择性可能是由于*CH插入甲酸盐形成乙酸盐所致,*CH是CO加氢制乙醇过程中的关键中间体。

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