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Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane

Author

Listed:
  • Junyan Zhang

    (Oak Ridge National Laboratory)

  • Yuanyuan Li

    (Oak Ridge National Laboratory)

  • Haohong Song

    (Vanderbilt University)

  • Lihua Zhang

    (Upton)

  • Yiqing Wu

    (Oak Ridge National Laboratory)

  • Yang He

    (Oak Ridge National Laboratory)

  • Lu Ma

    (Upton)

  • Jiyun Hong

    (SLAC National Accelerator Laboratory)

  • Akhil Tayal

    (Upton)

  • Nebojsa Marinkovic

    (Columbia University)

  • De-en Jiang

    (Vanderbilt University
    Vanderbilt University)

  • Zhenglong Li

    (Zhejiang University
    Institute of Zhejiang University)

  • Zili Wu

    (Oak Ridge National Laboratory
    Oak Ridge National Laboratory)

  • Felipe Polo-Garzon

    (Oak Ridge National Laboratory)

Abstract

Ni-based catalysts are highly reactive for dry reforming of methane (DRM) but they are prone to rapid deactivation due to sintering and/or coking. In this study, we present a straightforward approach for anchoring dispersed Ni sites with strengthened metal-support interactions, which leads to Ni active sites embedded in dealuminated Beta zeolite with superior stability and rates for DRM. The process involves solid-state grinding of dealuminated Beta zeolites and nickel nitrate, followed by calcination under finely controlled gas flow conditions. By combining in situ X-ray absorption spectroscopy and ab initio simulations, it is elucidated that the efficient removal of byproducts during catalyst synthesis is conducted to strengthen Ni–Si interactions that suppress coking and sintering after 100 h of time-on-stream. Transient isotopic kinetic experiments shed light on the differences in intrinsic turnover frequency of Ni species and explain performance trends. This work constructs a fundamental understanding regarding the implication of facile synthesis protocols on metal-support interaction in zeolite-supported Ni sites, and it lays the needed foundations on how these interactions can be tuned for outstanding DRM performance.

Suggested Citation

  • Junyan Zhang & Yuanyuan Li & Haohong Song & Lihua Zhang & Yiqing Wu & Yang He & Lu Ma & Jiyun Hong & Akhil Tayal & Nebojsa Marinkovic & De-en Jiang & Zhenglong Li & Zili Wu & Felipe Polo-Garzon, 2024. "Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50729-8
    DOI: 10.1038/s41467-024-50729-8
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    References listed on IDEAS

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    1. Y. Li & D. Zakharov & S. Zhao & R. Tappero & U. Jung & A. Elsen & Ph. Baumann & R.G. Nuzzo & E.A. Stach & A.I. Frenkel, 2015. "Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes," Nature Communications, Nature, vol. 6(1), pages 1-6, November.
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