期刊
CHEMICAL ENGINEERING JOURNAL
卷 433, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.134421
关键词
Hydrogen evolution reaction; Ruthenium nanoparticles; Ruthenium-oxygen bond; Activity; Stability
资金
- Hainan Province Science and Technology Special Fund [ZDYF2020037, ZDYF2020207]
- National Natural Science Foundation of China [21805104, 22109034, 22109035, 52164028, 62105083]
- Postdoctoral Science Foundation of Hainan Province [RZ2100007123]
- Basic and Applied Basic Research Foundation of Guangdong Province [2019A1515110558]
- Start-up Research Foundation of Hainan University [20082, KYQD(ZR)-20008, 20083, 20084, 21124, 21125]
In this study, reduced graphene oxide supported ruthenium nanoparticles catalysts were synthesized by annealing, and exhibited low overpotential and desirable stability in alkaline electrolytes. The introduction of oxygen-rich functional groups in graphene oxide improved the catalytic activity and stability of ruthenium catalysts by weakening the Ru-H affinity and strengthening the Ru-O bond.
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.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据