Self- regeneration of Au/CeO2 based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination

Lin Ye, Xinping Duan, Simson Wu, Tai-Sing Wu, Yuxin Zhao, Alex W. Robertson, Hung-Lung Chou, Jianwei Zheng, Tuğçe Ayvalı, Sarah Day, Chiu Tang, Yun-Liang Soo, Youzhu Yuan () and Shik Chi Edman Tsang ()
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Lin Ye: University of Oxford
Xinping Duan: Xiamen University
Simson Wu: University of Oxford
Tai-Sing Wu: National Tsing Hua University
Yuxin Zhao: Xiamen University
Alex W. Robertson: University of Oxford
Hung-Lung Chou: National Taiwan University of Science and Technology
Jianwei Zheng: University of Oxford
Tuğçe Ayvalı: University of Oxford
Sarah Day: Diamond Light Source Ltd, Harwell Science and Innovation Campus
Chiu Tang: Diamond Light Source Ltd, Harwell Science and Innovation Campus
Yun-Liang Soo: National Tsing Hua University
Youzhu Yuan: Xiamen University
Shik Chi Edman Tsang: University of Oxford

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Replacement of Hg with non-toxic Au based catalysts for industrial hydrochlorination of acetylene to vinyl chloride is urgently required. However Au catalysts suffer from progressive deactivation caused by auto-reduction of Au(I) and Au(III) active sites and irreversible aggregation of Au(0) inactive sites. Here we show from synchrotron X-ray absorption, STEM imaging and DFT modelling that the availability of ceria(110) surface renders Au(0)/Au(I) as active pairs. Thus, Au(0) is directly involved in the catalysis. Owing to the strong mediating properties of Ce(IV)/Ce(III) with one electron complementary redox coupling reactions, the ceria promotion to Au catalysts gives enhanced activity and stability. Total pre-reduction of Au species to inactive Au nanoparticles of Au/CeO2&AC when placed in a C2H2/HCl stream can also rapidly rejuvenate. This is dramatically achieved by re-dispersing the Au particles to Au(0) atoms and oxidising to Au(I) entities, whereas Au/AC does not recover from the deactivation.

Date: 2019
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DOI: 10.1038/s41467-019-08827-5

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