Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 32, Pages 13423-13429Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202005930
Keywords
ammonia; electrocatalysis; nitrogen reduction; single-atom catalysts
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Funding
- Natural Science Foundation of China [51432009, 11874334, 51872292]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2020458]
- CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
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Single-atom catalysts have demonstrated their superiority over other types of catalysts for various reactions. However, the reported nitrogen reduction reaction single-atom electrocatalysts for the nitrogen reduction reaction exclusively utilize metal-nitrogen or metal-carbon coordination configurations as catalytic active sites. Here, we report a Fe single-atom electrocatalyst supported on low-cost, nitrogen-free lignocellulose-derived carbon. The extended X-ray absorption fine structure spectra confirm that Fe atoms are anchored to the support via the Fe-(O-C-2)(4) coordination configuration. Density functional theory calculations identify Fe-(O-C-2)(4) as the active site for the nitrogen reduction reaction. An electrode consisting of the electrocatalyst loaded on carbon cloth can afford a NH3 yield rate and faradaic efficiency of 32.1 mu g h(-1) mg(cat.)(-1) (5350 mu g h(-1) mg(Fe)(-1)) and 29.3 %, respectively. An exceptional NH3 yield rate of 307.7 mu g h(-1) mg(cat.)(-1) (51 283 mu g h(-1) mg(Fe)(-1)) with a near record faradaic efficiency of 51.0 % can be achieved with the electrocatalyst immobilized on a glassy carbon electrode.
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