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

Author

Listed:
  • 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)

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.

Suggested Citation

  • 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 & Shik Chi Edman , 2019. "Self- regeneration of Au/CeO2 based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08827-5
    DOI: 10.1038/s41467-019-08827-5
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    Cited by:

    1. Yurui Fan & Haomiao Xu & Guanqun Gao & Mingming Wang & Wenjun Huang & Lei Ma & Yancai Yao & Zan Qu & Pengfei Xie & Bin Dai & Naiqiang Yan, 2024. "Asymmetric Ru-In atomic pairs promote highly active and stable acetylene hydrochlorination," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Gui Zhao & Jiayi Lin & Mengying Lu & Lina Li & Pengtao Xu & Xi Liu & Liwei Chen, 2024. "Potential cycling boosts the electrochemical conversion of polyethylene terephthalate-derived alcohol into valuable chemicals," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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