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

来源：

JOURNAL OF CATALYSIS | 2011年 / 283卷 / 01期

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

页码：89 / 97

页数：9

共 40 条

[11]

BROWN JHC, 1981, SYNTHESIS-STUTTGART, P441

[12] SOLUBILITY OF HYDROGEN IN 10 ORGANIC-SOLVENTS AT 298.15-K, 323.15-K, AND 373.15-K [J].

BRUNNER, E .

JOURNAL OF CHEMICAL AND ENGINEERING DATA, 1985, 30 (03) :269-273

[13] Monolayer bimetallic surfaces: Experimental and theoretical studies of trends in electronic and chemical properties [J].

Chen, Jingguang G. ;

Menning, Carl A. ;

Zellner, Michael B. .

SURFACE SCIENCE REPORTS, 2008, 63 (05) :201-254

[14]

Dobson I. D., 1988, Patent, Patent No. [0286280, EP0286280]

[15] Influence of the oxidative/reductive treatments on the activity of Pt/Ce0.67Zr0.33O2 catalyst [J].

Fan, J ;

Wu, XD ;

Ran, R ;

Weng, DA .

APPLIED SURFACE SCIENCE, 2005, 245 (1-4) :162-171

[16] Information on alpha-norlupinone - Its reduction into norlupinane. [J].

Galinovsky, F ;

Stern, E .

BERICHTE DER DEUTSCHEN CHEMISCHEN GESELLSCHAFT, 1943, 76 :1034-1038

[17] UBER DIE KATALYTISCHE REDUKTION ALIPHATISCHER CARBONSAUREAMIDE [J].

GUYER, A ;

BIELER, A ;

GERLICZY, G .

HELVETICA CHIMICA ACTA, 1955, 38 (06) :1649-1654

[18] Hydrogenation of amides by the use of bimetallic catalysts consisting of Group 8 to 10, and Group 6 or 7 metals [J].

Hirosawa, C ;

Wakasa, N ;

Fuchikami, T .

TETRAHEDRON LETTERS, 1996, 37 (37) :6749-6752

[19] A TEMPERATURE PROGRAMMED REDUCTION STUDY OF PT ON AL2O3 AND TIO2 [J].

HUIZINGA, T ;

VANGRONDELLE, J ;

PRINS, R .

APPLIED CATALYSIS, 1984, 10 (02) :199-213

[20] SOLUBILITIES OF HYDROGEN AND NITROGEN IN ALCOHOLS AND NORMAL-HEXANE [J].

KATAYAMA, T ;

NITTA, T .

JOURNAL OF CHEMICAL AND ENGINEERING DATA, 1976, 21 (02) :194-196

← 1 2 3 4 →