期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 7, 期 34, 页码 19977-19983出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta07790a
关键词
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资金
- NSFC [51672011]
- Guangdong Natural Science Funds for Distinguished Young Scholar [2015A030306036]
- Shenzhen Science and Technology Innovation Committee [JCYJ20170303140959031, JCYJ20180302150402760]
The electrochemical N-2 reduction reaction (NRR) in an aqueous medium has recently aroused great attention for the synthesis of NH3 under ambient conditions. However, this process generally suffers from a low NH3 production rate and often requires a noble-metal based electrocatalyst with some sophisticated nanosynthesis method. This work reports a new non-precious, self-supportive iron sulfide (FeSx) NRR electrocatalyst, synthesized by a simple H2S-plasma treatment on low-cost Fe foam. The H2S-plasma treatment sulfurizes the Fe surface to afford a self-supportive FeSx thin layer on the Fe foam (FeSx/Fe). The synthesized FeSx/Fe foam can be directly used as the electrode for the NRR, and it is demonstrated to show a remarkable NH3 production rate of 4.13 x 10(-10) mol s(-1) cm(-2) and a high faradaic efficiency of 17.6%, significantly outperforming many other reported non-precious electrocatalysts. Further material characterization shows that the surface FeSx converts to the mackinawite FeS after the NRR; the mackinawite FeS is possibly the actual high-activity NRR electrocatalyst, and density functional theory calculation is further employed to elucidate the NRR mechanism. Given the high performance and low cost, we envision that the plasma-synthesized FeSx/Fe will be of great promise for the electrochemical NH3 synthesis under ambient conditions.
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