Isolating the contributions of surface Sn atoms in the bifunctional behaviour of PtSn CO oxidation electrocatalysts
Isolating the contributions of surface Sn atoms in the bifunctional behaviour of PtSn CO oxidation electrocatalysts
Authors (4): H. Huang, O. F. Blackman, V. Celorrio, A. E. Russell
Themes: BAG
DOI: 10.1016/j.electacta.2021.138811
Citations: 14
Pub type: journal-article
Pub year: 2021

Publisher: Elsevier BV

Issue:

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Publication date(s): 2021/09 (online)

Pages: 138811

Volume: 390 Issue:

Journal: NA

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URL: http://dx.doi.org/10.1016/j.electacta.2021.138811

The bifunctional mechanism is well-acknowledged for the promoted CO oxidation on Pt-based bimetallic electrocatalysts. However, the direct identification of the active oxygenated species and the nature and electrochemistry of the second component are still a matter of debate. Herein, Snad-Pt/C catalysts, where Sn ad-atoms are exclusively on the surface of Pt nanoparticles at low coverages ranging from 0.0033 to 0.2 monolayers to avoid sub-surface Sn and alloy formation, were prepared as a model system to resolve these issues using a surface organometallic chemistry approach. Effects of the Sn ad-atoms on CO oxidation were studied by CO stripping voltammograms as a function of Sn coverage. Using in situ XAS measurements, the Sn average oxidation state is estimated to increase from +0.2 to +3.1 as the potential increases from 0 to 0.8 VRHE, with the number of the oxygen neighbours increasing stepwise. Pt4.5-Sn-(OH)1.5 is revealed as the active species responsible for the bifunctional mechanism at low overpotentials and is generated via a redox couple corresponding to Pt4.5-Sn*/Pt4.5-Sn-(OH)1.5.

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