期刊
NANO RESEARCH
卷 13, 期 5, 页码 1376-1382出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-020-2637-8
关键词
P-doped carbon nanotubes; nitrogen reduction reaction; active sites; reaction pathway; electrocatalysis
The electrochemical nitrogen reduction reaction (NRR) as an energy-efficient approach for ammonia synthesis is hampered by the low ammonia yield and ambiguous reaction mechanism. Herein, phosphorus-doped carbon nanotube (P-CNTs) is developed as an efficient metal-free electrocatalyst for NRR with a remarkable NH3 yield of 24.4 mu g center dot h(-1)center dot mg(cat.)(-1) and partial current density of 0.61 mA center dot cm(-2). Such superior activity is found to be from P doping and highly conjugated CNTs substrate. Experimental and theoretical investigations discover that the electron-deficient phosphorus sites with Lewis acidity should be genuine active sites and NRR on P-CNTs follows the distal pathway. These findings provide insightful understanding on NRR processes on P-CNTs, opening up opportunities for the rational design of highly-active cost-effective metal-free catalysts for electrochemical ammonia synthesis.
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