Catalytic hydrogenation of tertiary amides at low temperatures and pressures using bimetallic Pt/Re-based catalysts

被引:112
作者
Burch, R. [1 ]
Paun, C. [1 ]
Cao, X. -M. [1 ]
Crawford, P. [1 ]
Goodrich, P. [1 ]
Hardacre, C. [1 ]
Hu, P. [1 ]
McLaughlin, L. [1 ]
Sa, J. [1 ]
Thompson, J. M. [1 ]
机构
[1] Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland
基金
英国工程与自然科学研究理事会;
关键词
Platinum; Rhenium; Bimetallic; Titania; Amide; DFT; DENSITY-FUNCTIONAL THEORY; SELECTIVE HYDROGENATION; REDUCTION; PLATINUM; DIBORANE; SURFACES; ALCOHOLS; METALS; AMINES; ACID;
D O I
10.1016/j.jcat.2011.07.007
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:89 / 97
页数:9
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