Effect of crystal facets in plasmonic catalysis
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 () and
Emiliano Cortés ()
Additional contact information
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
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
Nature Communications, 2024, vol. 15, issue 1, 1-13
Abstract:
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.
Date: 2024
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47994-y
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DOI: 10.1038/s41467-024-47994-y
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