1. ·H effectively enhance electrocatalytic nitrogen fixation.
- Author
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Sun, Yuyao, Yu, Yaodong, Xu, Wenxia, Wu, Di, Wei, Yingying, Lai, Jianping, and Wang, Lei
- Subjects
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ELECTRON paramagnetic resonance , *FOURIER transform infrared spectroscopy , *NITROGEN fixation , *HYDROGEN evolution reactions , *NUCLEAR magnetic resonance , *ELECTROLYTE solutions - Abstract
We report for the first time the application of ·H for electrocatalytic N 2 reduction reaction (NRR). ·H from H 2 O can effectively lower the reaction energy barrier, and inhibit HER in electrocatalytic NRR, which expect also be used in other electrocatalytic fields where water is involved as well. [Display omitted] • ·H is applied for the first time in the fields of NRR. • This catalyst achieves the high ammonia yield of 100.7 ug h−1 mg cat −1 with ·H. • The in situ FTIR/ESR/DFT show that ·H from H 2 O effectively lowered the reaction energy barrie and inhibits HER. Nowadays, most reported ammonia (NH 3) yields and Faradaic efficiency (FE) of electrocatalysts are very low in the field of electrocatalytic nitrogen reduction reactions (NRR). Here, we are reported ·H for the first time in the field of electrocatalytic NRR, which are generated by sulfite (SO 3 2−) and H 2 O in electrolyte solutions upon exposure to UV light. The high NH 3 yields can achieve 100.7 μg h−1 mg cat −1, while stability can achieve 64 h and the FE can achieve 27.1% at −0.3 V (vs. RHE) with UV irradiation. In situ Fourier transform infrared spectroscopy (FTIR), electron spin resonance (ESR), density functional theory (DFT) and 1H nuclear magnetic resonance (NMR) tests showed that the ∙H effectively lowered the reaction energy barrier at each step of the NRR process and inhibits the occurrence of competitive hydrogen evolution reaction (HER). This explores the path and provides ideas for the field of electrocatalysis involving water. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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