Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (1): 98-106.

Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation

Hongpeng Zhang, Haichao Liu*

Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Stable and Unstable Species, College of Chemistry and
Molecular Engineering, Peking University, Beijing 100871, China

收稿日期:2012-06-05 修回日期:2012-08-11 出版日期:2013-01-20 发布日期:2013-02-06
通讯作者: 刘海超
基金资助:
国家自然科学基金;国家重点基础研究发展计划(973计划)

Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation

Hongpeng Zhang, Haichao Liu*

Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Stable and Unstable Species, College of Chemistry and
Molecular Engineering, Peking University, Beijing 100871, China

Received:2012-06-05 Revised:2012-08-11 Online:2013-01-20 Published:2013-02-06
Supported by:
;National Basic Research Program of China (973 Program)

摘要/Abstract

摘要： Au/Ce_1-xZr_xO₂ catalysts (x = 0--0.8) were prepared by a deposition-precipitation method using Ce_1-xZr_xO₂ nanoparticles as supports with variable Ce and Zr contents. Their structures were characterized by complimentary means such as X-ray diffraction, Raman, scanning transmission electron microscopy and X-ray photoelectron spectroscopy (XPS). These Au catalysts possessed similar sizes and crystalline phases of Ce_1-xZr_xO₂ supports as well as similar sizes and oxidation states of Au nanoparticles. The oxidation state of Au nanoparticles was dominated by Au⁰ especially in CO oxidation. Their activities were examined in CO oxidation at different temperatures in the range of 303-333 K. The CO oxidation rates normalized per Au atoms increased with the increasing Ce contents, and reached the maximum value over Au/CeO₂. Such change was in parallel with the change in the oxygen storage capacity values, i.e. the amounts of active oxygen species on Au/Ce_1-xZr_xO₂ catalysts. The excellent correlation between the two properties of the catalysts suggests that the intrinsic support effects on the CO oxidation rates is related to the effects on the adsorption and activation of O₂ on Au/Ce_1-xZr_xO₂ catalysts. Such understanding on the support effects may be useful for designing more active Au catalysts, for example, by tuning the redox properties of oxide supports.

关键词: gold catalyst, ceria-zirconia support, CO oxidation, oxygen storage capacity, support effect

Abstract: Au/Ce_1-xZr_xO₂ catalysts (x = 0--0.8) were prepared by a deposition-precipitation method using Ce_1-xZr_xO₂ nanoparticles as supports with variable Ce and Zr contents. Their structures were characterized by complimentary means such as X-ray diffraction, Raman, scanning transmission electron microscopy and X-ray photoelectron spectroscopy (XPS). These Au catalysts possessed similar sizes and crystalline phases of Ce_1-xZr_xO₂ supports as well as similar sizes and oxidation states of Au nanoparticles. The oxidation state of Au nanoparticles was dominated by Au⁰ especially in CO oxidation. Their activities were examined in CO oxidation at different temperatures in the range of 303-333 K. The CO oxidation rates normalized per Au atoms increased with the increasing Ce contents, and reached the maximum value over Au/CeO₂. Such change was in parallel with the change in the oxygen storage capacity values, i.e. the amounts of active oxygen species on Au/Ce_1-xZr_xO₂ catalysts. The excellent correlation between the two properties of the catalysts suggests that the intrinsic support effects on the CO oxidation rates is related to the effects on the adsorption and activation of O₂ on Au/Ce_1-xZr_xO₂ catalysts. Such understanding on the support effects may be useful for designing more active Au catalysts, for example, by tuning the redox properties of oxide supports.

Key words: gold catalyst, ceria-zirconia support, CO oxidation, oxygen storage capacity, support effect

Hongpeng Zhang, Haichao Liu* . Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation[J]. 能源化学(英文), 2013, 22(1): 98-106.

Hongpeng Zhang, Haichao Liu* . Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation[J]. Journal of Energy Chemistry, 2013, 22(1): 98-106.

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Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation

Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation

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