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论文编号: 122214O120120280
第一作者所在部门: 609组
中文论文题目: Ga-Pd/Ga2O3 Catalysts: The Role of Gallia Polymorphs,Intermetallic Compounds, and Pretreatment Conditions on Selectivity and Stability in Different Reactions
英文论文题目: Ga-Pd/Ga2O3 Catalysts: The Role of Gallia Polymorphs,Intermetallic Compounds, and Pretreatment Conditions on Selectivity and Stability in Different Reactions
论文题目英文:
作者: 李连地
论文出处:
刊物名称: Chem Cat Chem
: 2012
:
: 4
: 1764-1775
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影响因子: 5.207
摘要: A series of gallia-supported Pd-Ga catalysts that consist of metallic nanoparticles on three porous polymorphs of Ga2O3 (a-, b- , and g-Ga2O3) were synthesized by a controlled co-precipitation of Pd and Ga. The effects of formation of Ga-Pd intermetallic compounds (IMCs) were studied in four catalytic reactions: methanol steam reforming, hydrogenation of acetylene, and methanol synthesis by CO and CO2 hydrogenation reactions. The IMC Pd2Ga forms upon reduction of a- and b-Ga2O3- supported materials in hydrogen at temperatures of 250 and 310 8C, respectively. At higher temperatures, Ga-enrichment of the intermetallic particles is observed, leading to formation of Pd5Ga3 before the support itself is reduced at temperatures above 5658C. In the case of Ga-Pd/g-Ga2O3, no information about the metal particles could be obtained owing to their very small size and high dispersion; however, the catalytic results suggest that the IMC Pd2Ga also forms in this sample.Pd2Ga/gallia samples show a stable selectivity towards ethylene in acetylene hydrogenation (75 %), which is higher than for a monometallic Pd reference catalyst. An even higher selectivity of 80% was observed for Pd5Ga3 supported on a-Ga2O3. In methanol steam reforming, the Ga-Pd/Gallia catalysts showed, in contrast to Pd/Al2O3, selectivity towards CO2 of up to 40 %. However, higher selectivities, which have been reported for Pd2Ga in literature, could not be reproduced in this study, which might be a result of particle size effects. The initially higher selectivity of the Pd5Ga3-containing samples was not stable, suggesting superior catalytic properties for this IMC, but that re-oxidation of Ga species and formation of Pd2Ga occurs under reaction conditions. In methanol synthesis, CO hydrogenation did not occur, but a considerable methanol yield from a CO2/H2 feed was observed for Pd2Ga/a-Ga2O3.
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