摘要
Electronic coupling with the support plays a crucial role in boosting the intrinsic catalytic activity of a single-atom catalyst.Herein,the three-dimensional(3D)hierarchical Co(OH)F nanosheet arrays modified by singleatom Ru(SA-Ru/Co(OH)F)are prepared by a facile one-step hydrothermal method under mild conditions,which exhibit excellent activity with an overpotential of 200 and 326 mV at 10 and 500 mA cm^(−2),respectively,as well as robust stability for oxygen evolution reaction(OER)in 1.0 mol L^(−1)KOH electrolyte.The study of electronic structures and surface chemical states before and after OER testing reveals that the strong electronic coupling between single-atom Ru and Co(OH)F induces the charge redistribution in SA-Ru/Co(OH)F and suppresses the excessive oxidation of Ru into higher valence state(more than+4)under high OER potential.This work provides a strategy to stabilize single-atom Ru by Co(OH)F that can enhance the activity and durability for OER under large current densities.
单原子与基底之间的电子耦合在提升单原子催化剂的本征催化活性方面起到至关重要的作用.本文通过一步水热法在温和条件下制备了单原子Ru修饰的三维多级Co(OH)F纳米片阵列催化剂.该催化剂在1 mol L^(−1)KOH电解液中展现出高的电催化析氧反应活性和稳定性,在10和500 mA cm^(−2)的电流密度下分别表现出200和326 mV的过电位.通过对催化剂析氧反应前后的电子结构和表面化学态的研究发现,单原子Ru和Co(OH)F之间强烈的电子耦合诱导体系电荷重新分布,并抑制了Ru在高的OER电势下被过度氧化为过高的价态(大于+4价).本工作提供了一个通过羟基氟化钴稳定单原子Ru,以提高大电流下析氧反应的活性和稳定性的策略.
作者
Shizheng Zhou
Haeseong Jang
Qing Qin
Zijian Li
Min Gyu Kim
Chuang Li
Xien Liu
Jaephil Cho
周士正;Haeseong Jang;秦清;李子健;Min Gyu Kim;李创;刘希恩;Jaephil Cho(State Key Laboratory Base of Eco-Chemical Engineering,College of Chemical Engineering,Qingdao University of Science and Technology,Qingdao 266042,China;Department of Energy Engineering,Department of Energy and Chemical Engineering,Ulsan National Institute of Science and Technology(UNIST),Ulsan 44919,South Korea;Department of Chemistry,City University of Hong Kong,Hong Kong,China;Beamline Research Division,Pohang Accelerator Laboratory(PAL),Pohang 37673,South Korea)
基金
Taishan Scholar Program of Shandong Province,China(ts201712045)
Shandong Provincial Key Research and Development Program(2019GGX102069)
the Natural Science Foundation of Shandong Province of China(ZR2018BB008)
Doctoral Found of Qingdao University of Science and Technology(0100229001 and 010029081)
2019 Research Funds of Ulsan National Institute of Science and Technology,South Korea(1.190002.01).
