Wu Jiandong, Fan Jinchang, Zhao Xiao, Wang Ying, Wang Dewen, Liu Hongtai, Gu Lin, Zhang Qinghua, Zheng Lirong, Singh David J, Cui Xiaoqiang, Zheng Weitao
State Key Laboratory of Automotive Simulation and Control, School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Jilin University, Changchun, 130012, China.
Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Laboratory of Advanced Materials and Electron Microscopy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
Angew Chem Int Ed Engl. 2022 Aug 22;61(34):e202207512. doi: 10.1002/anie.202207512. Epub 2022 Jul 11.
Accelerating slow water dissociation kinetics is key to boosting the hydrogen evolution reaction (HER) in alkaline media. We report the synthesis of atomically dispersed MoO species anchored on Rh metallene using a one-pot solvothermal method. The resulting structures expose the oxide-metal interfaces to the maximum extent. This leads to a MoO -Rh catalyst with ultrahigh alkaline HER activity. We obtained a mass activity of 2.32 A mg at an overpotential of 50 mV, which is 11.8 times higher than that of commercial Pt/C and surpasses the previously reported Rh-based electrocatalysts. First-principles calculations demonstrate that the interface between MoO and Rh is the active center for alkaline HER. The MoO sites preferentially adsorb and dissociate water molecules, and adjacent Rh sites adsorb the generated atomic hydrogen for efficient H evolution. Our findings illustrate the potential of atomic interface engineering strategies in electrocatalysis.
加速缓慢的水电离动力学是促进碱性介质中析氢反应（HER）的关键。我们报道了使用一锅溶剂热法合成锚定在Rh金属烯上的原子分散的MoO物种。所得结构最大程度地暴露了氧化物-金属界面。这导致了具有超高碱性HER活性的MoO-Rh催化剂。我们在50 mV的过电位下获得了2.32 A mg的质量活性，这比商业Pt/C高11.8倍，并且超过了先前报道的Rh基电催化剂。第一性原理计算表明，MoO和Rh之间的界面是碱性HER的活性中心。MoO位点优先吸附和离解水分子，相邻的Rh位点吸附生成的原子氢以实现高效的氢析出。我们的研究结果说明了原子界面工程策略在电催化中的潜力。
