Lin Hao Yang, Yang Qian Qian, Lin Miao Yu, Xu Hao Guan, Tang Xuan, Fu Huai Qin, Wu Haoran, Zhu Minghui, Zhou Lihui, Yuan Hai Yang, Dai Sheng, Liu Peng Fei, Yang Hua Gui
Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai, 200237, China.
Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry & Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China.
Adv Mater. 2024 Oct;36(40):e2408045. doi: 10.1002/adma.202408045. Epub 2024 Aug 23.
Inefficient active site utilization of oxygen evolution reaction (OER) catalysts have limited the energy efficiency of proton exchange membrane (PEM) water electrolysis. Here, an atomic grid structure is demonstrated composed of high-density Ir sites (≈10 atoms per nm) on reactive MnO support which mediates oxygen coverage-enhanced OER process. Experimental characterizations verify the low-valent Mn species with decreased oxygen coordination in MnO exert a pivotal impact in the enriched oxygen coverage on the surface during OER process, and the distributed Ir atomic grids, where highly electrophilic Ir─O bonds proceed rapidly, render intense nucleophilic attack of oxygen radicals. Thereby, this metal-support cooperation achieves ultra-low overpotentials of 166 mV at 10 mA cm and 283 mV at 500 mA cm, together with a striking mass activity which is 380 times higher than commercial IrO at 1.53 V. Moreover, its high OER performance also markedly surpasses the commercial Ir black catalyst in PEM electrolyzers with long-term stability.
析氧反应(OER)催化剂活性位点利用效率低下限制了质子交换膜(PEM)水电解的能量效率。在此,展示了一种由活性MnO载体上的高密度Ir位点(约每纳米10个原子)组成的原子网格结构,该结构介导了氧覆盖增强的OER过程。实验表征证实,MnO中氧配位减少的低价Mn物种在OER过程中对表面富集的氧覆盖起关键作用,而分布的Ir原子网格中,高亲电性的Ir─O键快速进行,引发氧自由基的强烈亲核攻击。因此,这种金属-载体协同作用在10 mA cm时实现了166 mV的超低过电位,在500 mA cm时实现了283 mV的超低过电位,同时具有惊人的质量活性,在1.53 V时比商业IrO高380倍。此外,其高OER性能在具有长期稳定性的PEM电解槽中也明显超过了商业Ir黑催化剂。