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The adsorption/desorption behavior of sulfurspecies at the (111) surfaces of pure Pt and various Pt-basedbimetallic alloys, denoted as Pt3M (M = Co, Cu, Fe, Pd), wasinvestigated by electrochemical measurements and X-ray photo-electron spectroscopy (XPS). After the adsorption of elementalsulfur, the current responses characteristic of the adsorption/desorption of hydrogen and hydroxyl species at the sulfur-free bare(111) surfaces completely disappeared, and a doublet peakcorresponding to the elemental sulfur appeared in the S 2p regionof XPS spectra. The characteristic current responses graduallyrecovered, simultaneously with the decrease of the S 2p peak, byrepeating the potential cycling between −0.2 and 0.8 V vs Ag/AgCl, indicating the oxidative desorption of S species. Except forthe Pt3Pd(111) surface, in which Pd has a similar atomic radius to Pt and fully occupied 4d orbitals, the Pt3M(111) surfaces showedhigher oxidative desorption capability than those of the pure Pt(111) surface; electrochemically active surface area recovered at thePt3M(111) surfaces by fewer potential cycles than at the Pt(111) surface. Among the various factors, the downshift of the d-bandcenter due to the ligand effect of foreign metal and the electronic interaction between adsorbed S and Pt are the dominant factorspromoting the oxidative desorption of sulfur as well as the strain effect of foreign metal with an atomic radius smaller than Pt.

Rights:

• Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International
  

Keyword: fuel cell, electrocatalysts, sulfur poisoning

Date published: 2025-01-30

Publisher: American Chemical Society (ACS)

Journal:

• The Journal of Physical Chemistry C (ISSN: 19327447) vol. 129 issue. 4 p. 2122-2131

Funding:

• New Energy and Industrial Technology Development Organization JPNP20003

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1021/acs.jpcc.4c06652

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Updated at: 2025-12-15 13:08:16 +0900

Published on MDR: 2025-03-26 17:27:03 +0900