Yuan Bichen, Dang Qian, Liu Hai, Sendeku Marshet Getaye, Peng Jian, Fan Yameng, Cai Liang, Cao Aiqing, Chen Shiyao, Li Hui, Kuang Yun, Wang Fengmei, Sun Xiaoming
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, PR China.
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, PR China.
Nat Commun. 2025 May 17;16(1):4583. doi: 10.1038/s41467-025-59710-5.
Low-cost ruthenium-based catalysts with high activity have emerged as promising alternatives to iridium-based counterparts for acidic oxygen evolution reaction (OER) in proton exchange membrane water electrolyzers (PEMWE), but the poor stability under high current density remains as a key challenge. Here, we utilize the synergistic complementary strategy of introducing earth-abundant Mn and Nb dopants in ruthenium dioxide (RuO) for NbMnRuO nanoparticle electrocatalyst that exhibits a low overpotential of 209 mV at 10 mA cm and good stability of > 400 h at 0.2 A cm in 0.5 M HSO Significantly, a PEMWE device fabricated with NbMnRuO anode can operate continuously at least for 1000 h at 0.5 A cm with 59 μV h decay rate. Operando Raman spectroscopy analysis, differential electrochemical mass spectroscopy measurements, X-ray absorption spectroscopy analysis and theoretical calculations indicate that OER reaction on NbMnRuO primarily follows the adsorbate evolution mechanism with much favorable energy barrier accompanied by a locally passivated lattice oxygen mechanism (AEM-LPLOM) and the co-existed Nb and Mn in RuO crystal lattice could not only stabilize the lattice oxygen, but also relieve the valence state fluctuation of Ru site to stabilize the catalyst during the reaction.
低成本、高活性的钌基催化剂已成为质子交换膜水电解槽(PEMWE)中酸性析氧反应(OER)中铱基催化剂的有前途的替代品,但在高电流密度下稳定性较差仍是一个关键挑战。在此,我们采用在二氧化钌(RuO₂)中引入储量丰富的锰(Mn)和铌(Nb)掺杂剂的协同互补策略,制备了NbMnRuO纳米颗粒电催化剂,该催化剂在10 mA cm⁻²时具有209 mV的低过电位,在0.5 M H₂SO₄中0.2 A cm⁻²时具有大于400 h的良好稳定性。值得注意的是,用NbMnRuO阳极制备的PEMWE装置在0.5 A cm⁻²下可连续运行至少1000 h,衰减率为59 μV h⁻¹。原位拉曼光谱分析、差分电化学质谱测量、X射线吸收光谱分析和理论计算表明,NbMnRuO上的OER反应主要遵循吸附质演化机制,具有更有利的能垒,同时伴有局部钝化晶格氧机制(AEM-LPLOM),并且RuO晶格中共存的Nb和Mn不仅可以稳定晶格氧,还可以缓解Ru位点的价态波动,从而在反应过程中稳定催化剂。