Zhu Jiawei, Guo Yao, Liu Fang, Xu Hanwen, Gong Lei, Shi Wenjie, Chen Ding, Wang Pengyan, Yang Yue, Zhang Chengtian, Wu Jinsong, Luo Jiahuan, Mu Shichun
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, P. R. China.
Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Xianhu Hydrogen Valley, Foshan, 528200, P. R. China.
Angew Chem Int Ed Engl. 2021 May 25;60(22):12328-12334. doi: 10.1002/anie.202101539. Epub 2021 Mar 30.
Theoretical calculations unveil the charge redistribution over abundant interfaces and the enhanced electronic states of Ru/RuS heterostructure. The resulting surface electron-deficient Ru sites display optimized adsorption behavior toward diverse reaction intermediates, thereby reducing the thermodynamic energy barriers. Experimentally, for the first time the laminar Ru/RuS heterostructure is rationally engineered by virtue of the synchronous reduction and sulfurization under eutectic salt system. Impressively, it exhibits extremely high catalytic activity for both OER (201 mV @ 10 mA cm ) and HER (45 mV @ 10 mA cm ) in acidic media due to favorable kinetics and excellent specific activity, consequently leading to a terrific performance in acidic overall water splitting devices (1.501 V @ 10 mA cm ). The in-depth insight into the internal activity origin of interfacial effect could offer precise guidance for the rational establishment of hybrid interfaces.
理论计算揭示了Ru/RuS异质结构丰富界面上的电荷重新分布以及增强的电子态。由此产生的表面电子缺陷Ru位点对各种反应中间体表现出优化的吸附行为，从而降低了热力学能垒。在实验方面，首次通过共晶盐体系下的同步还原和硫化合理构建了层状Ru/RuS异质结构。令人印象深刻的是，由于良好的动力学和出色的比活性，它在酸性介质中对析氧反应（在10 mA cm时过电位为201 mV）和析氢反应（在10 mA cm时过电位为45 mV）均表现出极高的催化活性，进而在酸性全水解装置中展现出优异的性能（在10 mA cm时电压为1.501 V）。对界面效应内部活性起源的深入了解可为合理构建混合界面提供精确指导。
