Miao Xianbing, Zhang Lifu, Wu Liang, Hu Zhenpeng, Shi Lei, Zhou Shiming
Hefei National Laboratory for Physics Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
School of Physics, Nankai University, Tianjin, 300071, P. R. China.
Nat Commun. 2019 Aug 23;10(1):3809. doi: 10.1038/s41467-019-11789-3.
Development of highly active and durable oxygen-evolving catalysts in acid media is a major challenge to design proton exchange membrane water electrolysis for producing hydrogen. Here, we report a quadruple perovskite oxide CaCuRuO as a superior catalyst for acidic water oxidation. This complex oxide exhibits an ultrasmall overpotential of 171 mV at 10 mA cm, which is much lower than that of the state-of-the-art RuO. Moreover, compared to RuO, CaCuRuO shows a significant increase in mass activity by more than two orders of magnitude and much better stability. Density functional theory calculations reveal that the quadruple perovskite catalyst has a lower Ru 4d-band center relative to RuO, which effectively optimizes the binding energy of oxygen intermediates and thereby enhances the catalytic activity.
开发在酸性介质中具有高活性和耐久性的析氧催化剂是设计用于制氢的质子交换膜水电解的一项重大挑战。在此，我们报道一种四重钙钛矿氧化物CaCuRuO作为酸性水氧化的优异催化剂。这种复合氧化物在10 mA cm时表现出171 mV的超小过电位，远低于最先进的RuO。此外，与RuO相比，CaCuRuO的质量活性显著提高了两个多数量级，且稳定性更好。密度泛函理论计算表明，四重钙钛矿催化剂相对于RuO具有更低的Ru 4d带中心，这有效地优化了氧中间体的结合能，从而提高了催化活性。
