TY - JOUR
T1 - Tailoring the Oxygen Vacancy Distribution in Se-Doped RuOx to Enhance Its Stability in Acidic Water Electrolysis
AU - Yang, Yongping
AU - Wang, Shulin
AU - Zhang, Guikai
AU - Li, Xingyu
AU - Wu, Qikai
AU - Liu, Hao
AU - Deng, Ziliang
AU - Han, Xinyi
AU - Zhang, Shuailong
AU - Dong, Wenbo
AU - Song, Jiangnan
AU - Chen, Yabin
AU - Gao, Xiao
AU - Yang, Yao
AU - Dong, Juncai
AU - Cao, Liang
AU - Zhao, Zipeng
N1 - Publisher Copyright:
© 2025 Wiley-VCH GmbH.
PY - 2025/10/6
Y1 - 2025/10/6
N2 - Developing durable ruthenium (Ru)-based catalysts for proton exchange membrane water electrolyzer (PEMWE) remains challenging due to irreversible Ru dissolution and lattice oxygen instability. Although elemental doping is a general method to improve stability, it inadvertently induces oxygen vacancies (VOs), which are randomly distributed in the nanocatalyst. Notably, the impact of VO distribution on the stability of Ru-based catalysts remains unresolved. Herein, we synthesized the Se-doped Ru oxide via annealing the mixture of ruthenium (III) chloride and selenium (Se) in the air (Ur-Se-RuOx) with the presence of urea, showing the VOs distributed away from Se dopants, which is significantly different from the Se-doped Ru oxide synthesized without urea (Se-RuOx), showing VOs distributed relatively close to the Se dopants. The Ur-Se-RuOx demonstrates superior oxygen evolution reaction performance over Se-RuOx. Particularly, Ur-Se-RuOx delivers a low working voltage (1.62 V@1 A cm−2) and excellent durability (>1000 h@200 mA cm−2) in PEMWE tests. Experimental and theoretical results reveal that VOs engage in long-range cooperation with spatially decoupled Se dopants in Ur-Se-RuOx, synergistically enhancing reaction kinetics via an intramolecular oxygen coupling mechanism, while inhibiting the lattice oxygen mechanism and suppressing Ru dissolution, which demonstrates a new strategy to break the activity–stability trade-off in promising Ru-based catalysts.
AB - Developing durable ruthenium (Ru)-based catalysts for proton exchange membrane water electrolyzer (PEMWE) remains challenging due to irreversible Ru dissolution and lattice oxygen instability. Although elemental doping is a general method to improve stability, it inadvertently induces oxygen vacancies (VOs), which are randomly distributed in the nanocatalyst. Notably, the impact of VO distribution on the stability of Ru-based catalysts remains unresolved. Herein, we synthesized the Se-doped Ru oxide via annealing the mixture of ruthenium (III) chloride and selenium (Se) in the air (Ur-Se-RuOx) with the presence of urea, showing the VOs distributed away from Se dopants, which is significantly different from the Se-doped Ru oxide synthesized without urea (Se-RuOx), showing VOs distributed relatively close to the Se dopants. The Ur-Se-RuOx demonstrates superior oxygen evolution reaction performance over Se-RuOx. Particularly, Ur-Se-RuOx delivers a low working voltage (1.62 V@1 A cm−2) and excellent durability (>1000 h@200 mA cm−2) in PEMWE tests. Experimental and theoretical results reveal that VOs engage in long-range cooperation with spatially decoupled Se dopants in Ur-Se-RuOx, synergistically enhancing reaction kinetics via an intramolecular oxygen coupling mechanism, while inhibiting the lattice oxygen mechanism and suppressing Ru dissolution, which demonstrates a new strategy to break the activity–stability trade-off in promising Ru-based catalysts.
KW - Elemental doping
KW - Oxygen evolution reaction
KW - Oxygen vacancy distribution
KW - Proton exchange membrane water electrolyzer
KW - Ru-based catalyst
UR - https://www.scopus.com/pages/publications/105013771664
U2 - 10.1002/anie.202512848
DO - 10.1002/anie.202512848
M3 - Article
C2 - 40844244
AN - SCOPUS:105013771664
SN - 1433-7851
VL - 64
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 41
M1 - e202512848
ER -