期刊
CHEMICAL ENGINEERING JOURNAL
卷 411, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.128488
关键词
Ni3S2; Electrocatalysts; Oxygen evolution reaction; Surface reconstruction; Fluorination
资金
- National Natural Science Foundation of China [21838003, 51621002]
- Shanghai Scientific and Technological Innovation Project [18JC1410600]
- Fundamental Research Funds for the Central Universities [222201718002]
In this study, a novel fluorinated Ni3S2 nanoarray electrocatalyst was reported, exhibiting excellent electrochemical performance during the OER process. The electrocatalyst showed a larger electrochemical active surface area, better conductivity, and higher OER activity, resulting in lower overpotential and Tafel slope compared to most reported Ni3S2-based electrocatalysts. The activation of NiF bonds under OER process generated highly active Ni-OOH species, contributing to the acceleration of rate-determining step.
Developing efficient electrocatalysts to accelerate the rate-determining step of oxygen evolution reaction (OER) is a tough challenge to water electrolysis. Herein, we report a fluorinated Ni3S2 nanoarray electrocatalyst with Ni-F bonds enriched and low-crystalline ultrathin nanosheets on the surface, which are responsible for the rapid and deep electrochemical-transformation of active phase during OER process. Electrochemical characterizations indicate that the fluorinated Ni3S2 (F-Ni3S2) possesses a larger electrochemical active surface area, better conductivity and higher intrinsic OER activity (TOF) than the pristine Ni3S2. Consequently, the optimized F-Ni3S2 electrocatalyst shows a small overpotential of 239 mV at 10 mA cm(-2) with a low Tafel slope of 36 mV dec(-1), superior to most of reported Ni3S2-based electrocatalysts to date. Ex-situ structural analysis further reveals the NiF bonds can be easily activated with F loss under OER process, thus generating more highly active Ni-OOH species for accelerating rate-determining step (*O -> *OOH). This work expands fluorine chemistry applications in designing high-activity electrocatalysts for energy-conversion.
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