Importance of broken geometric symmetry of single-atom Pt sites for efficient electrocatalysis

Junsic Cho, Taejung Lim, Haesol Kim, Ling Meng, Jinjong Kim, Seunghoon Lee, Jong Hoon Lee, Gwan Yeong Jung, Kug-Seung Lee, Francesc Viñes, Francesc Illas, Kai S. Exner (), Sang Hoon Joo () and Chang Hyuck Choi ()
Additional contact information
Junsic Cho: Pohang University of Science and Technology (POSTECH)
Taejung Lim: Ulsan National Institute of Science and Technology (UNIST)
Haesol Kim: Pohang University of Science and Technology (POSTECH)
Ling Meng: Universitat de Barcelona, c/ Martí i Franquès 1-11
Jinjong Kim: Ulsan National Institute of Science and Technology (UNIST)
Seunghoon Lee: Pohang University of Science and Technology (POSTECH)
Jong Hoon Lee: Ulsan National Institute of Science and Technology (UNIST)
Gwan Yeong Jung: Ulsan National Institute of Science and Technology (UNIST)
Kug-Seung Lee: Pohang University of Science and Technology (POSTECH)
Francesc Viñes: Universitat de Barcelona, c/ Martí i Franquès 1-11
Francesc Illas: Universitat de Barcelona, c/ Martí i Franquès 1-11
Kai S. Exner: University of Duisburg-Essen, 45141 Essen, Germany; Cluster of Excellence RESOLV, 44801 Bochum, Germany; Center for Nanointegration Duisburg-Essen (CENIDE)
Sang Hoon Joo: Ulsan National Institute of Science and Technology (UNIST)
Chang Hyuck Choi: Pohang University of Science and Technology (POSTECH)

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Platinum single-atom catalysts hold promise as a new frontier in heterogeneous electrocatalysis. However, the exact chemical nature of active Pt sites is highly elusive, arousing many hypotheses to compensate for the significant discrepancies between experiments and theories. Here, we identify the stabilization of low-coordinated PtII species on carbon-based Pt single-atom catalysts, which have rarely been found as reaction intermediates of homogeneous PtII catalysts but have often been proposed as catalytic sites for Pt single-atom catalysts from theory. Advanced online spectroscopic studies reveal multiple identities of PtII moieties on the single-atom catalysts beyond ideally four-coordinated PtII–N4. Notably, decreasing Pt content to 0.15 wt.% enables the differentiation of low-coordinated PtII species from the four-coordinated ones, demonstrating their critical role in the chlorine evolution reaction. This study may afford general guidelines for achieving a high electrocatalytic performance of carbon-based single-atom catalysts based on other d8 metal ions.

Date: 2023
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DOI: 10.1038/s41467-023-38964-x

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