Eliminating dissolution of platinum-based electrocatalysts at the atomic scale

Pietro P Lopes; Dongguo Li; Haifeng Lv; Chao Wang; Dusan Tripkovic; Yisi Zhu; Roberto Schimmenti; Hideo Daimon; Yijin Kang; Joshua Snyder; Nigel Becknell; Karren L More; Dusan Strmcnik; Nenad M Markovic; Manos Mavrikakis; Vojislav R Stamenkovic

doi:10.1038/s41563-020-0735-3

Eliminating dissolution of platinum-based electrocatalysts at the atomic scale

Nat Mater. 2020 Nov;19(11):1207-1214. doi: 10.1038/s41563-020-0735-3. Epub 2020 Jul 20.

Authors

Pietro P Lopes¹, Dongguo Li¹, Haifeng Lv¹, Chao Wang², Dusan Tripkovic^{1

3}, Yisi Zhu¹, Roberto Schimmenti⁴, Hideo Daimon⁵, Yijin Kang¹, Joshua Snyder⁶, Nigel Becknell¹, Karren L More⁷, Dusan Strmcnik¹, Nenad M Markovic¹, Manos Mavrikakis⁴, Vojislav R Stamenkovic⁸

Affiliations

¹ Materials Science Division, Argonne National Laboratory, Lemont, IL, USA.
² Department of Chemical Engineering, John Hopkins University, Baltimore, MD, USA.
³ Faculty for Technology and Metallurgy, University of Belgrade, Belgrade, Serbia.
⁴ Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, WI, USA.
⁵ Faculty of Science and Engineering, Doshisha University, Kyoto, Japan.
⁶ Department of Chemical Engineering, Drexel University, Philadelphia, PA, USA.
⁷ Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, USA.
⁸ Materials Science Division, Argonne National Laboratory, Lemont, IL, USA. vrstamenkovic@anl.gov.

PMID: 32690912
DOI: 10.1038/s41563-020-0735-3

Abstract

A remaining challenge for the deployment of proton-exchange membrane fuel cells is the limited durability of platinum (Pt) nanoscale materials that operate at high voltages during the cathodic oxygen reduction reaction. In this work, atomic-scale insight into well-defined single-crystalline, thin-film and nanoscale surfaces exposed Pt dissolution trends that governed the design and synthesis of durable materials. A newly defined metric, intrinsic dissolution, is essential to understanding the correlation between the measured Pt loss, surface structure, size and ratio of Pt nanoparticles in a carbon (C) support. It was found that the utilization of a gold (Au) underlayer promotes ordering of Pt surface atoms towards a (111) structure, whereas Au on the surface selectively protects low-coordinated Pt sites. This mitigation strategy was applied towards 3 nm Pt₃Au/C nanoparticles and resulted in the elimination of Pt dissolution in the liquid electrolyte, which included a 30-fold durability improvement versus 3 nm Pt/C over an extended potential range up to 1.2 V.