期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 7, 期 46, 页码 26371-26377出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta10206j
关键词
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资金
- NSFC [21725101, 21871244, 21521001]
- Fundamental Research Funds for the Central Universities [WK2060030029]
- China Postdoctoral Science Foundation [2019TQ0298]
- Supercomputing Center of USTC
The electrocatalytic nitrogen reduction reaction (NRR) has much prospect for substituting the energy-consuming Haber-Bosch process. Nevertheless, its sluggish reaction kinetics and the competing hydrogen evolution reaction always result in limited ammonia yield and low faradaic efficiency (FE). In this work, an Fe-decorated porphyrinic metal-organic framework (MOF) is employed as a precursor to construct single-atom Fe implanted nitrogen-doped carbon catalysts (Fe-1-N-C) through a mixed ligand strategy. Benefiting from the highly dispersed single-atom Fe sites, hierarchically porous structure and good conductivity, Fe-1-N-C shows a FE of 4.51% and an ammonia yield rate of 1.56 x 10(-11) mol cm(-2) s(-1) at -0.05 V versus the reversible hydrogen electrode, superior to those of Co-1-N-C and Ni-1-N-C. Theoretical calculations reveal that Fe-1-N-C shows the lowest energy barrier of the rate-determining step during the NRR process, consistent with its highest activity obtained in experiments. This work reveals the unique potential of single-atom catalysts for the electrochemical NRR and provides in-depth insights into the catalytic mechanism of the NRR.
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