Regulating orbital interaction to construct quasi-covalent bond networks in Pt intermetallic alloys for high-performance fuel cells

Xuan Liu, Yuhan Wang, Hu He, Zhonglong Zhao (), Xuan Luo, Siyang Zhang, Gang Lu, Dong Su, Yucheng Wang (), Yunhui Huang and Qing Li ()
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Xuan Liu: Huazhong University of Science and Technology
Yuhan Wang: Chinese Academy of Sciences
Hu He: China Institute of Atomic Energy
Zhonglong Zhao: Inner Mongolia University
Xuan Luo: Xiamen University
Siyang Zhang: Huazhong University of Science and Technology
Gang Lu: California State University Northridge
Dong Su: Chinese Academy of Sciences
Yucheng Wang: Xiamen University
Yunhui Huang: Huazhong University of Science and Technology
Qing Li: Huazhong University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract The long-standing challenges facing Pt-based alloy catalysts in oxygen reduction reactions (ORRs) are rapid oxidation and loss of transition metal/Pt in proton exchange membrane fuel cells (PEMFCs). In this work, we report a concept of “covalentization” in intermetallic L10-PtMM’ (M = Fe, Co, Ni and M’ = one of the 4th-period elements (from Ti to Ge)) alloys to enhance their electrochemical stability. Specifically, the formation of a quasi-covalent bond network in L10-PtMM’ due to the less occupied antibonding states induced by high d-band positions of M’ elements (e.g., Ti, V, Cr) enhances atomic bond order and strength, diminishing Co anodic dissolution via strengthened Pt/Co-M’ bonds and reducing Co cathodic corrosion by inhibiting Pt oxidation through an electron buffering effect. The developed L10-PtCoCr/C catalysts show a high mass activity (MA = 1.27 A mgPt−1) and rated power (16.5 W mgPt−1) in PEMFCs at a low total Pt loading of 0.075 mgPt cm−2. The catalysts also exhibit high electrochemical stability with ~3% and 5% loss of MA and rated power after 30,000 accelerated durability testing cycles and projects a lifetime of about 42,000 hours.

Date: 2025
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DOI: 10.1038/s41467-025-60171-z

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