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Elucidating the mechanism of heterogeneous Wacker oxidation over Pd-Cu/zeolite Y by transient XAS

Author

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  • Jerick Imbao

    (Paul Scherrer Institute
    ETH Zurich, Institute for Chemical and Bioengineering)

  • Jeroen A. Bokhoven

    (Paul Scherrer Institute
    ETH Zurich, Institute for Chemical and Bioengineering)

  • Adam Clark

    (Paul Scherrer Institute)

  • Maarten Nachtegaal

    (Paul Scherrer Institute)

Abstract

The heterogenization of Wacker catalysts using chloride-free systems can potentially be a good alternative for the commercial homogeneous Wacker oxidation of ethylene, which utilizes excessive aqueous chloride solvents. However, the mechanism of the heterogeneous system has not been clarified, preventing the rational design of better catalysts. Here, we report a transient X-ray absorption spectroscopic (XAS) investigation of the heterogeneous Wacker oxidation over Pd-Cu/zeolite Y coupled with kinetic studies and chemometric analysis. Insight is obtained by operando quickXAS allowing the quantitative determination of rates and thereby revealing a rapid redox reaction involving copper. Our work demonstrates that copper is not only the site of oxygen activation, but is also involved in the formation of undesired carbon dioxide. Without detecting the presence of Cu(0) and Pd(I), our results suggest that two one-electron transfers to two Cu(II) ions to reoxidize Pd(0) is at work in this heterogeneous Wacker catalyst.

Suggested Citation

  • Jerick Imbao & Jeroen A. Bokhoven & Adam Clark & Maarten Nachtegaal, 2020. "Elucidating the mechanism of heterogeneous Wacker oxidation over Pd-Cu/zeolite Y by transient XAS," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-14982-x
    DOI: 10.1038/s41467-020-14982-x
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    Cited by:

    1. Xingpeng Li & Hongzhe Jiang & Xuesong Jiang & Minghong Shi, 2021. "Identification of Geographical Origin of Chinese Chestnuts Using Hyperspectral Imaging with 1D-CNN Algorithm," Agriculture, MDPI, vol. 11(12), pages 1-19, December.

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