Methyl Formate Formation from Methanol Oxidation Using Supported Gold-Palladium Nanoparticles

被引:94
作者
Whiting, Gareth T. [1 ]
Kondrat, Simon A. [1 ]
Hammond, Ceri [1 ]
Dimitratos, Nikolaos [1 ]
He, Qian [2 ]
Morgan, David J. [1 ]
Dummer, Nicholas F. [1 ]
Bartley, Jonathan K. [1 ]
Kiely, Christopher J. [2 ]
Taylor, Stuart H. [1 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, Wales
[2] Lehigh Univ, Dept Mat Sci & Engn, Bethlehem, PA 18015 USA
来源
ACS CATALYSIS | 2015年 / 5卷 / 02期
基金
英国工程与自然科学研究理事会;
关键词
methanol; methyl formate; oxidation; gold-palladium; nanoparticles; active species; SOLVENT-FREE OXIDATION; SELECTIVE OXIDATION; CATALYTIC-ACTIVITY; ALCOHOL OXIDATION; OXIDE CATALYSTS; FUEL PROPERTIES; CO OXIDATION; FT-IR; ADSORPTION; OXYGEN;
D O I
10.1021/cs501728r
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
Recent advances in the oxidation of alcohols to methyl esters using metal nanoparticles have paved the way for more environmentally benign processes, operating at lower reaction temperatures with high product selectivity. Here, we demonstrate the use of bimetallic I wt % Au-Pd/TiO2 catalysts that achieve high activity for the oxidation of methanol to methyl formate at low temperature. The application of a water extraction treatment to retain size-stabilized Au-Pd nanoparticles, in contrast to a more standard thermal treatment, provides the most active catalyst for this reaction. Using in situ DRIFTS, we demonstrate that in situ activation during methanol oxidation enhances the catalytic activity at low temperature and that this is a long-lived effect. Surface adsorbates, particularly formate species, build up on the catalyst surface during the reaction and are proven vital to enhancing the catalytic effect.
引用
收藏
页码:637 / 644
页数:8
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