Methanol synthesis from CO2 and H2 using supported Pd alloy catalysts

被引:14
作者
Lawes, Naomi [1 ]
Gow, Isla E. [1 ]
Smith, Louise R. [1 ]
Aggett, Kieran J. [1 ]
Hayward, James S. [1 ]
Kabalan, Lara [1 ]
Logsdail, Andrew J. [1 ]
Slater, Thomas J. A. [1 ]
Dearg, Malcolm [1 ]
Morgan, David J. [1 ]
Dummer, Nicholas F. [1 ]
Taylor, Stuart H. [1 ]
Bowker, Michael [1 ]
Catlow, C. Richard A. [1 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Max Planck Cardiff Ctr Fundamentals Heterogeneous, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, Wales
基金
英国工程与自然科学研究理事会;
关键词
ATMOSPHERIC-PRESSURE; CARBON-DIOXIDE; HYDROGENATION;
D O I
10.1039/d2fd00119e
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
A number of Pd based materials have been synthesised and evaluated as catalysts for the conversion of carbon dioxide and hydrogen to methanol, a useful platform chemical and hydrogen storage molecule. Monometallic Pd catalysts show poor methanol selectivity, but this is improved through the formation of Pd alloys, with both PdZn and PdGa alloys showing greatly enhanced methanol productivity compared with monometallic Pd/Al2O3 and Pd/TiO2 catalysts. Catalyst characterisation shows that the 1 : 1 beta-PdZn alloy is present in all Zn containing post-reaction samples, including PdZn/Ga2O3, with the Pd2Ga alloy formed for the Pd/Ga2O3 sample. The heat of mixing was calculated for a variety of alloy compositions with high values determined for both PdZn and Pd2Ga alloys, at ca. -0.6 eV per atom and ca. -0.8 eV per atom, respectively. However, ZnO is more readily reduced than Ga2O3, providing a possible explanation for the preferential formation of the PdZn alloy, rather than PdGa, when in the presence of Ga2O3.
引用
收藏
页码:193 / 211
页数:19
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