Catalytic hydrogenation of tertiary amides at low temperatures and pressures using bimetallic Pt/Re-based catalysts
Catalytic hydrogenation of tertiary amides at low temperatures and pressures using bimetallic Pt/Re-based catalysts
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DOI：
10.1016/j.jcat.2011.07.007
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发表时间：
2011-10-06
影响因子：
7.3
通讯作者：
Thompson, J. M.
中科院分区：
文献类型：
--
作者：
Burch, R.;Paun, C.;Thompson, J. M.
TiO（2）负载的Pt/Re催化剂可在低温和低压下有效地促进叔酰胺，特别是N-甲基吡咯烷-2-酮的加氢。表征的催化剂和动力学测试表明，密切的相互作用之间的Re和Pt是至关重要的高活性观察。DFT计算被用来检查的范围内的金属组合，并表明，未配位的Re的作用是激活的C=O和Pt的是作为一种加氢催化剂，从催化剂表面除去中间体。在TiO（2）载体上观察到的速率增强被认为是由于氧空位的存在允许吸附和削弱C=O键。(C)2011 Elsevier Inc. All rights reserved.
Hydrogenation of tertiary amides, in particular, N-methylpyrrolidin-2-one, can be efficiently facilitated by a TiO(2)-supported bimetallic Pt/Re catalyst at low temperatures and pressures. Characterisation of the catalysts and kinetic tests have shown that the close interaction between the Re and Pt is crucial to the high activity observed. DFT calculations were used to examine a range of metal combinations and show that the role of the uncoordinated Re is to activate the C=O and that of the Pt is as a hydrogenation catalyst, removing intermediates from the catalyst surface. The rate enhancement observed on the TiO(2) support is thought to be due to the presence of oxygen vacancies allowing adsorption and weakening of the C=O bond. (C) 2011 Elsevier Inc. All rights reserved.