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Critical surface strain regime for stable and active epitaxial platinum oxygen reduction electrocatalysts

delete2026-07-02
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PRE
AI
Z
Zhenhua Zeng *
G
Guangdong Liu
D
David A. Cullen
H
Huiqiu Deng
A
Andrew J. Steinbach *
G
Grant M. Thoma
A
A. Jeremy Kropf
D
Deborah J. Myers
Z
Zhongxia Shang
F
Fumiharu Kusaka
N
Naoto Todoroki
J
Jeffrey P. Greeley
DOI:10.1038/s41560-026-02108-4delete
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Abstract

Abstract

En 中文
Manipulating surface strain via lattice mismatch can enhance electrocatalytic activity in epitaxial transition metal films, but long-term performance remains challenging. Although thick films can improve stability against dissolution, they may suffer from irreversible strain relaxation, reducing catalytic activity. Here using epitaxial platinum films for the electrochemical oxygen reduction reaction, we demonstrate thickness-dependent critical strain below which irreversible strain relaxation is avoided, defining the thicknesses range that optimizes catalyst stability and activity. First principles calculations reveal that the critical strain values range from −8.2% (compressive) to 2.7% (tensile) and the optimal strain (−2.5%) is maintained in Pt films up to ~3-nm thick. In H2–air polymer electrolyte membrane fuel cells, Pt films on iridium deliver a mass activity of 1.5 ± 0.3 A mgPt−1 at 0.9 V and less than 10% performance loss after 30,000 cycles, compared with less than 0.4 A mgPt−1 and more than 60% performance loss for Pt and PtNi catalysts. Manipulating surface strain in epitaxial transition metal films can enhance electrocatalytic activity, yet maintaining long-term performance is challenging due to irreversible strain relaxation. Here the authors identify a thickness-dependent critical strain in epitaxial Pt/Ir films that optimizes stability and activity for the oxygen reduction reaction.

Journal

Nature Energy cover
Nature Energy
IF:
60.1
Papers:
981
Citations:
5.6W

Organization

3
3m company
Scholars:
20
Papers: 7
Citations: 0
U
University of Wisconsin–Madison
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732
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T
Tohoku University
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P
Purdue University
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H
hunan university
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O
oak ridge national laboratory
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1.4W
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A
argonne national laboratory
Scholars:
643
Papers: 260
Citations: 0
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