Bridge the activity and durability of Ruthenium for hydrogen evolution reaction with the Ru-O-C link

被引：41

作者：

Yang, Yingjie ^{[1
]}

Wu, Daoxiong ^{[1
]}

Yu, Yanhui ^{[1
]}

Li, Jing ^{[1
]}

Rao, Peng ^{[1
]}

Jia, Chunman ^{[1
]}

Liu, Zhongxin ^{[1
]}

Chen, Qi ^{[1
]}

Huang, Wei ^{[1
]}

Luo, Junming ^{[1
]}

Deng, Peilin ^{[1
]}

Shen, Yijun ^{[1
]}

Tian, Xinlong ^{[1
]}

机构：

[1] Hainan Univ, State Key Lab Marine Resource Utilizat South Chin, Hainan Prov Key Lab Fine Chem, Sch Chem Engn & Technol, Haikou 570228, Hainan, Peoples R China

来源：

CHEMICAL ENGINEERING JOURNAL | 2022年 / 433卷

基金：

中国国家自然科学基金;

关键词：

Hydrogen evolution reaction; Ruthenium nanoparticles; Ruthenium-oxygen bond; Activity; Stability; TOTAL-ENERGY CALCULATIONS; PLANE-WAVE; EFFICIENT; NANOPARTICLES; OXIDATION; CATALYST; CRYSTAL;

D O I：

10.1016/j.cej.2021.134421

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Exploring efficient and robust electrocatalysts with low cost for hydrogen evolution reaction (HER) is critical for the practical application of electrochemical water splitting. Ruthenium (Ru)-based catalysts exhibit great po-tential in HER, whereas the extensive application is largely hampered by the insufficient performance and durability at current stage. In addition, understanding and revealing the activity enhancement mechanism of Ru-based catalysts is still very tempting while challenging. Herein, we use the oxygen-rich functional groups of graphene oxide (GO) to adsorb Ru species and in situ generate reduced graphene oxide supported Ru nano-particles (NPs) catalysts by annealing (Ru/rGO-700). Ru/rGO-700 exhibits low overpotential of 26 mV at 10 mA cm-2 in alkaline electrolytes, and simultaneously the strong interaction induced by the Ru-O bond between the support and the anchored Ru NPs endows the catalyst a desirable stability, thus the activity of the catalysts barely decays after 50,000 cycles of durability testing. Density functional theory (DFT) calculations demonstrate that the introduction of anionic oxygen leads to the electron-deficient characteristics of Ru NPs, which weakens the Ru-H affinity and accelerates/ or favors water dissociation and hydrogen desorption. In addition, the integrated crystal orbital Hamilton population (ICOHP) confirms that the introduction of electron holes weakens the an-tibonding interactions between Ru atoms, thus the stability of the catalysts is greatly improved.

引用

页数：7

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