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Reaction heat-driven CO2 desorption during CO oxidation on Au(997) at low temperatures

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Abstract

Adsorption and reaction of CO and CO2 were studied on oxygen-covered Au(997) surfaces by means of temperatureprogrammed desorption/reaction spectroscopy. Oxygen atoms (O(a)) on Au(997) enhances the CO2 adsorption and stabilizes the adsorbed CO2(a), and the stabilization effect also depends on the CO2(a) coverage and involved Au sites. CO2(a) desorption is the rate-limiting step for the CO+O(a) reaction to produce CO2 on Au(997) at 105 K and exhibits complex behaviors, including the desorption of CO2(a) upon CO exposures at 105 K and the desorption of O(a)-stabilized CO2(a) at elevated temperatures. The desorption of CO2(a) from the surface upon CO exposures at 105 K to produce gaseous CO2 depends on the surface reaction extent and involves the reaction heat-driven CO2(a) desorption channel. CO+O(a) reaction proceeds more easily with weakly-bound oxygen adatoms at the (111) terraces than strongly-bound oxygen adatoms at the (111) steps. These results reveal complex rate-limiting CO2(a) desorption behaviors during CO+O(a) reaction on Au surfaces at low temperatures which provide novel information on the fundamental understanding of Au catalysis.

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Authors and Affiliations

  1. Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China

    Zongfang Wu, Zhiquan Jiang, Yuekang Jin, Feng Xiong, Guanghui Sun & Weixin Huang

  2. CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei, 230026, China

    Zongfang Wu, Zhiquan Jiang, Yuekang Jin, Feng Xiong, Guanghui Sun & Weixin Huang

  3. Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China

    Zongfang Wu, Zhiquan Jiang, Yuekang Jin, Feng Xiong, Guanghui Sun & Weixin Huang

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  1. Zongfang Wu
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  2. Zhiquan Jiang
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  3. Yuekang Jin
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  5. Guanghui Sun
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  6. Weixin Huang
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Correspondence to Weixin Huang.

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Wu, Z., Jiang, Z., Jin, Y. et al. Reaction heat-driven CO2 desorption during CO oxidation on Au(997) at low temperatures. Sci. China Chem. 59, 752–759 (2016). https://doi.org/10.1007/s11426-015-5510-y

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  • DOI: https://doi.org/10.1007/s11426-015-5510-y

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