TY - JOUR
T1 - Intrinsic Ferromagnetism Coupling-Driven the Spin Reconfiguration of Single-Atom Ru for Enhanced Acidic Water Oxidation
AU - Jin, Jing
AU - Liu, Yifan
AU - Liu, Zhihang
AU - Peng, Xing
AU - Li, Yingqiang
AU - Hao, Libin
AU - Liu, Chao
AU - Zhang, Wenyao
AU - Fu, Yongsheng
AU - Jiang, Xiaohong
AU - Xiong, Pan
AU - Zhu, Junwu
N1 - Publisher Copyright:
© 2025 Wiley-VCH GmbH.
PY - 2025
Y1 - 2025
N2 - Oxygen evolution reaction (OER) is essential for electrochemical water splitting and renewable hydrogen production. Ruthenium-based catalysts exhibit excellent performance but suffer from insufficient stability to practical application. Herein, a spin-state engineering strategy is explored to modulate the spin-electron distribution of Ru single atoms via the intrinsic magnetism of Mn5O8 substrate for efficient acidic OER. In Ru─Mn5O8 system, the favorable Ru4+-O-Mn2+ configuration facilitates Ru-site spin polarization and drives Ru4+ from low-spin to high-spin through strong ferromagnetic coupling, whereas Ru4+ remains low-spin in nonferromagnetic Ru─MnO2. Unpaired dπ electrons of high-spin Ru4+ enhance π-donation to coordinated O2−, optimizing Ru─O orbital overlap. Moreover, the interaction between high-spin Ru4+ and key intermediates is strengthened. Consequently, Ru─Mn5O8 achieves a low overpotential of 186 mV at 10 mA cm−2 and sustains stability over 160 h at 100 mA cm−2 in acidic medium, outperforming Ru─MnO2 (440 mV, 30 h) and commercial RuO2 (250 mV, 40 h). When applied as an anode in a proton exchange membrane water electrolyzer, Ru─Mn5O8 realizes 1 A cm−2 at 1.68 V and maintains stable operation for over 50 h. This work proposes a ferromagnetic interaction-driven spin modulation strategy, offering a robust pathway for designing high-performance electrocatalysts for acidic water oxidation.
AB - Oxygen evolution reaction (OER) is essential for electrochemical water splitting and renewable hydrogen production. Ruthenium-based catalysts exhibit excellent performance but suffer from insufficient stability to practical application. Herein, a spin-state engineering strategy is explored to modulate the spin-electron distribution of Ru single atoms via the intrinsic magnetism of Mn5O8 substrate for efficient acidic OER. In Ru─Mn5O8 system, the favorable Ru4+-O-Mn2+ configuration facilitates Ru-site spin polarization and drives Ru4+ from low-spin to high-spin through strong ferromagnetic coupling, whereas Ru4+ remains low-spin in nonferromagnetic Ru─MnO2. Unpaired dπ electrons of high-spin Ru4+ enhance π-donation to coordinated O2−, optimizing Ru─O orbital overlap. Moreover, the interaction between high-spin Ru4+ and key intermediates is strengthened. Consequently, Ru─Mn5O8 achieves a low overpotential of 186 mV at 10 mA cm−2 and sustains stability over 160 h at 100 mA cm−2 in acidic medium, outperforming Ru─MnO2 (440 mV, 30 h) and commercial RuO2 (250 mV, 40 h). When applied as an anode in a proton exchange membrane water electrolyzer, Ru─Mn5O8 realizes 1 A cm−2 at 1.68 V and maintains stable operation for over 50 h. This work proposes a ferromagnetic interaction-driven spin modulation strategy, offering a robust pathway for designing high-performance electrocatalysts for acidic water oxidation.
KW - ferromagnetic interaction
KW - oxygen evolution reaction
KW - proton exchange membrane water electrocatalysis
KW - single atoms
KW - spin-state
UR - https://www.scopus.com/pages/publications/105022684687
U2 - 10.1002/adfm.202525644
DO - 10.1002/adfm.202525644
M3 - 文章
AN - SCOPUS:105022684687
SN - 1616-301X
JO - Advanced Functional Materials
JF - Advanced Functional Materials
ER -
