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Interplay between copper redox and transfer and support acidity and topology in low temperature NH3-SCR

Author

Listed:
  • Yiqing Wu

    (Pacific Northwest National Laboratory)

  • Wenru Zhao

    (Tiangong University)

  • Sang Hyun Ahn

    (Division of Environmental Science and Engineering, POSTECH)

  • Yilin Wang

    (Pacific Northwest National Laboratory)

  • Eric D. Walter

    (Pacific Northwest National Laboratory)

  • Ying Chen

    (Pacific Northwest National Laboratory)

  • Miroslaw A. Derewinski

    (Pacific Northwest National Laboratory
    Polish Academy of Sciences)

  • Nancy M. Washton

    (Pacific Northwest National Laboratory)

  • Kenneth G. Rappé

    (Pacific Northwest National Laboratory)

  • Yong Wang

    (Pacific Northwest National Laboratory
    Washington State University)

  • Donghai Mei

    (Tiangong University
    Tiangong University)

  • Suk Bong Hong

    (Division of Environmental Science and Engineering, POSTECH)

  • Feng Gao

    (Pacific Northwest National Laboratory)

Abstract

Low-temperature standard NH3-SCR over copper-exchanged zeolite catalysts occurs on NH3-solvated Cu-ion active sites in a quasi-homogeneous manner. As key kinetically relevant reaction steps, the reaction intermediate CuII(NH3)4 ion hydrolyzes to CuII(OH)(NH3)3 ion to gain redox activity. The CuII(OH)(NH3)3 ion also transfers between neighboring zeolite cages to form highly reactive reaction intermediates. Via operando electron paramagnetic resonance spectroscopy and SCR kinetic measurements and density functional theory calculations, we demonstrate here that such kinetically relevant steps become energetically more difficult with lower support Brønsted acid strength and density. Consequently, Cu/LTA displays lower Cu atomic efficiency than Cu/CHA and Cu/AEI, which can also be rationalized by considering differences in their support topology. By carrying out hydrothermal aging to eliminate support Brønsted acid sites, both CuII(NH3)4 ion hydrolysis and CuII(OH)(NH3)3 ion migration are hindered, leading to a marked decrease in Cu atomic efficiency for all catalysts.

Suggested Citation

  • Yiqing Wu & Wenru Zhao & Sang Hyun Ahn & Yilin Wang & Eric D. Walter & Ying Chen & Miroslaw A. Derewinski & Nancy M. Washton & Kenneth G. Rappé & Yong Wang & Donghai Mei & Suk Bong Hong & Feng Gao, 2023. "Interplay between copper redox and transfer and support acidity and topology in low temperature NH3-SCR," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38309-8
    DOI: 10.1038/s41467-023-38309-8
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    References listed on IDEAS

    as
    1. Paolo Cleto Bruzzese & Enrico Salvadori & Stefan Jäger & Martin Hartmann & Bartolomeo Civalleri & Andreas Pöppl & Mario Chiesa, 2021. "17O-EPR determination of the structure and dynamics of copper single-metal sites in zeolites," Nature Communications, Nature, vol. 12(1), pages 1-13, December.
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