Research Article


2016, 9(12): 3868–3880


New mechanistic pathways for CO oxidation catalyzed by single-atom catalysts: Supported and doped Au1/ThO2

Bo Long1,2, Yan Tang1, and Jun Li1 (*)

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1 Department of Chemistry and Laboratory of Organic Optoelectronics & Molecular Engineering of the Ministry of Education, Tsinghua University, Beijing 100084, China
2 College of Information Engineering, Guizhou Minzu University, Guiyang 550025, China

Keywords: CO oxidation, single gold catalysis, catalytic mechanism, actinide oxides
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ABSTRACT Single-atom catalysts are of great interest and importance for designing new high-performance low-cost catalysts. We investigated CO oxidation catalyzed by single gold atoms supported on thoria (Au/ThO2) and doped ThO2 using density functional theory with Hubbard-type on-site Coulomb interaction (DFT + U). The calculation results show that the Au-doped ThO2(111) catalyst exhibits remarkable catalytic activity for CO oxidation via the Eley–Rideal mechanism in three steps, where the rate-determining step is decomposition of the OCOO* intermediate with an energy barrier of 0.58 eV. Moreover, our results also reveal a new mechanism of CO oxidation on a gold adatom supported by ThO2(111), where O2 is adsorbed only at the Th site on the surface, and the gas-phase CO then reacts directly with the activated O2 * to form CO2, which is the rate-limiting step, with a barrier of 0.46 eV. It is found that CO oxidation can occur without CO and O2 coadsorption on Au, which was previously considered a key intermediate. Therefore, these results provide new insights into CO oxidation on isolated gold atoms supported by the 5f-element compound ThO2(111). This mechanism can help clarify the catalytic cycle of CO oxidation, support the design of highperformance low-cost catalysts, and elucidate the redox properties of actinide oxides.
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New mechanistic pathways for CO oxidation catalyzed by single-atom catalysts: Supported and doped Au1/ThO2. Nano Res. 2016, 9(12): 3868–3880

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