Hu Wei, Huang Bolong, Sun Mingzi, Du Jing, Hai Yang, Yin Wen, Wang Xiaomei, Gao Wensheng, Zhao Chunyang, Yue Ya, Li Zelong, Li Can
Key Laboratory of Advanced Catalysis, Gansu province, State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, Gansu, 730000, China.
Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, 100872, China.
Adv Mater. 2025 Jan;37(3):e2411709. doi: 10.1002/adma.202411709. Epub 2024 Nov 30.
The development of efficient and durable electrocatalysts for the acidic oxygen evolution reaction (OER) is essential for advancing renewable hydrogen energy technology. However, the slow deprotonation kinetics of oxo-intermediates, involving the four proton-coupled electron steps, hinder the acidic OER progress. Herein, a RuTiO solid solution electrocatalyst is investigated, which features bridged oxygen (O) sites that act as proton acceptors, accelerating the deprotonation of oxo-intermediates. Electrochemical tests, infrared spectroscopy, and density functional theory results reveal that the moderate proton adsorption energy on O sites facilitates fast deprotonation kinetics through the adsorbate evolution mechanism. This process effectively prevents the over-oxidation and deactivation of Ru sites caused by the lattice oxygen mechanism. Consequently, RuTiO shows a low overpotential of 198 mV at 10 mA cm and performance exceeding 1400 h at 50 mA cm with negligible deactivation. These insights into the OER mechanism and the structure-function relationship are crucial for the advancement of catalytic systems.
开发高效耐用的酸性析氧反应(OER)电催化剂对于推动可再生氢能技术至关重要。然而,涉及四个质子耦合电子步骤的氧代中间体的缓慢去质子动力学阻碍了酸性OER的进展。在此,研究了一种RuTiO固溶体电催化剂,其具有充当质子受体的桥连氧(O)位点,加速了氧代中间体的去质子化。电化学测试、红外光谱和密度泛函理论结果表明,O位点上适度的质子吸附能通过吸附质演化机制促进了快速去质子动力学。该过程有效地防止了由晶格氧机制引起的Ru位点的过度氧化和失活。因此,RuTiO在10 mA cm 时显示出198 mV的低过电位,在50 mA cm 时性能超过1400 h,失活可忽略不计。这些对OER机制和结构-功能关系的见解对于催化系统的发展至关重要。