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Effect of crystal facets in plasmonic catalysis

Author

Listed:
  • Yicui Kang

    (Ludwig-Maximilians-Universität München)

  • Simão M. João

    (Imperial College London)

  • Rui Lin

    (Ludwig-Maximilians-Universität München)

  • Kang Liu

    (Central South University)

  • Li Zhu

    (Ludwig-Maximilians-Universität München)

  • Junwei Fu

    (Central South University)

  • Weng-Chon (Max) Cheong

    (University of Science and Technology)

  • Seunghoon Lee

    (Ludwig-Maximilians-Universität München
    Dong-A University
    Dong-A University)

  • Kilian Frank

    (Ludwig-Maximilians-Universität)

  • Bert Nickel

    (Ludwig-Maximilians-Universität)

  • Min Liu

    (Central South University)

  • Johannes Lischner

    (Imperial College London)

  • Emiliano Cortés

    (Ludwig-Maximilians-Universität München)

Abstract

While the role of crystal facets is well known in traditional heterogeneous catalysis, this effect has not yet been thoroughly studied in plasmon-assisted catalysis, where attention has primarily focused on plasmon-derived mechanisms. Here, we investigate plasmon-assisted electrocatalytic CO2 reduction using different shapes of plasmonic Au nanoparticles - nanocube (NC), rhombic dodecahedron (RD), and octahedron (OC) - exposing {100}, {110}, and {111} facets, respectively. Upon plasmon excitation, Au OCs doubled CO Faradaic efficiency (FECO) and tripled CO partial current density (jCO) compared to a dark condition, with NCs also improving under illumination. In contrast, Au RDs maintained consistent performance irrespective of light exposure, suggesting minimal influence of light on the reaction. Temperature experiments ruled out heat as the main factor to explain such differences. Atomistic simulations and electromagnetic modeling revealed higher hot carrier abundance and electric field enhancement on Au OCs and NCs than RDs. These effects now dominate the reaction landscape over the crystal facets, thus shifting the reaction sites when comparing dark and plasmon-activated processes. Plasmon-assisted H2 evolution reaction experiments also support these findings. The dominance of low-coordinated sites over facets in plasmonic catalysis suggests key insights for designing efficient photocatalysts for energy conversion and carbon neutralization.

Suggested Citation

  • Yicui Kang & Simão M. João & Rui Lin & Kang Liu & Li Zhu & Junwei Fu & Weng-Chon (Max) Cheong & Seunghoon Lee & Kilian Frank & Bert Nickel & Min Liu & Johannes Lischner & Emiliano Cortés, 2024. "Effect of crystal facets in plasmonic catalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47994-y
    DOI: 10.1038/s41467-024-47994-y
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    References listed on IDEAS

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    4. Min Liu & Yuanjie Pang & Bo Zhang & Phil De Luna & Oleksandr Voznyy & Jixian Xu & Xueli Zheng & Cao Thang Dinh & Fengjia Fan & Changhong Cao & F. Pelayo García de Arquer & Tina Saberi Safaei & Adam Me, 2016. "Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration," Nature, Nature, vol. 537(7620), pages 382-386, September.
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