Mixed-Dimensional Partial Dealloyed PtCuBi/C as High-Performance Electrocatalysts for Methanol Oxidation with Enhanced CO Tolerance

Sichen Li; Sara Ajmal; Xiaoxing Zhou; Maoni Lu; Xinghao Li; Zhenjie Sun; Shoujie Liu; Manzhou Zhu; Peng Li

doi:10.1002/smll.202309226

Mixed-Dimensional Partial Dealloyed PtCuBi/C as High-Performance Electrocatalysts for Methanol Oxidation with Enhanced CO Tolerance

Small. 2023 Dec 21:e2309226. doi: 10.1002/smll.202309226. Online ahead of print.

Authors

Sichen Li¹, Sara Ajmal¹, Xiaoxing Zhou¹, Maoni Lu¹, Xinghao Li¹, Zhenjie Sun¹, Shoujie Liu², Manzhou Zhu¹, Peng Li¹

Affiliations

¹ Department of Chemistry and Center for Atomic Engineering of Advanced Materials, School of Materials Science and Engineering, Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Anhui University, Hefei, 230601, P. R. China.
² School of Materials Science and Engineering, Anhui University, Hefei, 230601, P. R. China.

PMID: 38126680
DOI: 10.1002/smll.202309226

Abstract

Developing efficient electrocatalysts for methanol oxidation reaction (MOR) is crucial in advancing the commercialization of direct methanol fuel cells (DMFCs). Herein, carbon-supported 0D/2D PtCuBi/C (0D/2D PtCuBi/C) catalysts are fabricated through a solvothermal method, followed by a partial electrochemical dealloying process to form a novel mixed-dimensional electrochemically dealloyed PtCuBi/C (0D/2D D-PtCuBi/C) catalysts. Benefiting from distinctive mixed-dimensional structure and composition, the as-obtained 0D/2D D-PtCuBi/C catalysts possess abundant accessible active sites. The introduction of Cu as a water-activating element weakens the CO_ads , and oxophilic metal Bi facilitates the OH_ads , thereby enhancing its tolerance to CO poisoning and promoting MOR activity. The X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure spectroscopy (XAFS) collectively reveal the electron transfer from Cu and Bi to Pt, the electron-enrichment effect induced by dealloying, and the strong interactions among Pt-M (Cu, Pt, and Bi) multi-active sites, which improve the tuning of the electronic structure and enhancement of electron transfer ability. Impressively, the optimized 0D/2D D-PtCuBi/C catalysts exhibit the superior mass activity (MA) of 17.68 A mg_Pt ^-1 for MOR, which is 14.86 times higher than that of commercial Pt/C. This study offers a proposed strategy for Pt-based alloy catalysts, enabling their use as efficient anodic materials in fuel cell applications.

Keywords: PtCuBi/C alloy electrocatalysts; element-specific; methanol oxidation reaction; mixed-dimensional; partial electrochemical dealloying.

Abstract

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