Citation: Ruyan Liu, Zhenrui Ni, Olim Ruzimuradov, Khayit Turayev, Tao Liu, Luo Yu, Panyong Kuang. Ni-induced modulation of Pt 5d-H 1s antibonding orbitals for enhanced hydrogen evolution and urea oxidation[J]. Acta Physico-Chimica Sinica, ;2025, 41(12): 100159. doi: 10.1016/j.actphy.2025.100159 shu

Ni-induced modulation of Pt 5d-H 1s antibonding orbitals for enhanced hydrogen evolution and urea oxidation

Ruyan Liu ^{1, †} ,
Zhenrui Ni ^{1, †} ,
Olim Ruzimuradov ^{2, 3} ,
Khayit Turayev ⁴ ,
Tao Liu ¹ ,
Luo Yu ¹ ,
Panyong Kuang ^1,,

1.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, 68 Jincheng Street, Wuhan 430078, Hubei Province, China
2.
Alfraganus University, Yuqori Karakamish Street 2a, Tashkent 100190, Uzbekistan
3.
Turin Polytechnic University in Tashkent, Kichik khalqa yoli 17, Tashkent 100095, Uzbekistan
4.
Termez State University, Barkamol Avlod Street 43, Termez 190111, Uzbekistan

Corresponding author: Panyong Kuang, kuangpanyong@cug.edu.cn

^†

Received Date: 24 July 2025
Revised Date: 12 August 2025
Accepted Date: 14 August 2025

Fund Project: the National Key Research and Development Program of China 2022YFB3803600National Natural Science Foundation of China 22272153National Natural Science Foundation of China 22479132National Natural Science Foundation of China 22238009National Natural Science Foundation of China U23A20102National Natural Science Foundation of China 22361142704National Natural Science Foundation of China 22309168the Natural Science Foundation of Hubei Province of China 2022CFA001Key R&D Program Projects in Hubei Province 2023BAB113

While H₂ features high energy density, environmental friendliness, and renewability, its efficient production is limited by the sluggish kinetics of the oxygen evolution reaction (OER). Here, we report a Pt@PtNi₃ core@shell alloy electrocatalyst that, through Ni incorporation, modulates the occupancy of Pt 5d antibonding orbitals and simultaneously enhances both hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) activities. The optimized Pt@PtNi₃-500 delivers an ultralow overpotential of 21 mV at 10 mA cm^-2 for HER under acidic conditions and a low onset potential of 1.27 V for UOR under alkaline conditions, surpassing monometallic Pt and Ni counterparts. When employed in an asymmetric acid-alkaline electrolyzer (HER/UOR), Pt@PtNi₃-500 achieves a 68.3% reduction in electrical energy consumption for H₂ production compared to traditional alkaline water splitting (HER/OER). Mechanistic investigations reveal that appropriate Ni incorporation in Pt@PtNi₃ increases the occupancy of Pt 5d–H 1s antibonding orbitals, which not only reinforces H⁺ adsorption but also weakens the overly strong H^* binding. Simultaneously, it reduces the energy barrier for ^*NH₂ dehydrogenation, thereby synergistically accelerating both H₂ generation and urea decomposition. This work provides new insights into the design of alloy electrocatalysts for high-efficiency H₂ production.
- Hydrogen evolution reaction,
- Urea oxidation reaction,
- Pt@PtNi₃ core@shell alloy,
- Asymmetric acid-alkaline catalysis,
- Antibonding orbital occupancy
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沈阳化工大学材料科学与工程学院沈阳 110142