Regulative Electronic States around Ruthenium/Ruthenium Disulphide Heterointerfaces for Efficient Water Splitting in Acidic Media

Regulative Electronic States around Ruthenium/Ruthenium Disulphide Heterointerfaces for Efficient Water Splitting in Acidic Media
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钌/二硫化钌异质界面周围的调节电子态,用于酸性介质中高效水分解

DOI:
10.1002/anie.202101539
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发表时间:
2021
期刊:
Angew. Chem. Int. Ed.
影响因子:
--
通讯作者:
Shichun Mu
Shichun Mu
中科院分区:
其他
文献类型:
--
作者:
Jiawei Zhu;Yao Guo;Fang Liu;Hanwen Xu;Lei Gong;Wenjie Shi;Ding Chen;Pengyan Wang;Yue Yang;Chengtian Zhang;Jinsong Wu;Jiahuan Luo;Shichun Mu

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理论计算揭示了Ru/RuS 2异质结构中电荷在丰富界面上的重新分布和电子态的增强。由此产生的表面缺电子Ru位点显示出对不同反应中间体的优化吸附行为,从而降低了热力学能垒。在实验上,首次通过共晶盐体系下的同步还原和硫化,实现了Ru/RuS 2层状异质结构的合理设计。令人印象深刻的是,由于有利的动力学和优异的比活性,它在酸性介质中对OER(201mV@10 mA cm−2)和HER(45 mV@10 mA cm−2)表现出极高的催化活性,从而在酸性整体水裂解装置中产生极好的性能(1.501 V@10 mA cm −2)。      深入了解界面效应的内在活动根源,可以为合理建立混合界面提供精确的指导。
Theoretical calculations unveil the charge redistribution over abundant interfaces and the enhanced electronic states of Ru/RuS2heterostructure. 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/RuS2heterostructure 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−2) and HER (45 mV @ 10 mA cm−2) 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−2). The in‐depth insight into the internal activity origin of interfacial effect could offer precise guidance for the rational establishment of hybrid interfaces.