Shape Effect of Pd-Promoted Ga2O3 Nanocatalysts for Methanol Synthesis by CO2 Hydrogenation

被引:77
|
作者
Qu, Jin [1 ,2 ,3 ]
Zhou, Xiwen [3 ]
Xu, Feng [3 ]
Gong, Xue-Qing [1 ,2 ]
Tsang, Shik Chi Edman [3 ]
机构
[1] E China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China
[2] E China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China
[3] Univ Oxford, Dept Chem, Wolfson Catalysis Ctr, Oxford OX1 3QR, England
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2014年 / 118卷 / 42期
基金
英国工程与自然科学研究理事会;
关键词
METAL-SUPPORT INTERACTION; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; COPPER-BASED CATALYSTS; CARBON-DIOXIDE; SELECTIVE HYDROGENATION; CU-ZNO/ZRO2; CATALYSTS; PALLADIUM CATALYSTS; ACTIVE-SITE; SURFACE;
D O I
10.1021/jp5063379
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
In this paper, we present a new approach to investigate metalsupport interaction in catalysis. First, we have carried out a controlled growth of two semiconductive Ga2O3 nanocrystals in distinctive shapes, namely, plate and rod with the majority of their surfaces covered with polar and nonpolar facets, respectively. We have then placed the same contents of Pd on these nanocrystals and carried out a systematic testing and characterization for methanol synthesis from CO2 hydrogenation under industrial applicable conditions. It is found that a low indexed (002) polar Ga2O3 surface is highly unstable, which gives oxygen defects and mobile electrons in the conduction band more readily than those nonpolar (111) and (110) surfaces. A significantly strong metalsupport interaction between the (002) polar Ga2O3 surface and Pd was determined, and it gave rise to higher metal dispersion and facilitated electron transfer between them, leading to the formation of PdGax. This renders such composite nanocatalysts active for methanol production.
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页码:24452 / 24466
页数:15
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