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Research Article

Phosphorus-doping activates carbon nanotubes for efficient electroreduction of nitrogen to ammonia

Lu-Pan Yuan1,2, Ze-Yuan Wu1,2, Wen-Jie Jiang1( ), Tang Tang1,2, Shuai Niu1,2, Jin-Song Hu1,2( )
Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
University of Chinese Academy of Sciences, Beijing 100049, China
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Abstract

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 μg·h-1·mg-1cat. and partial current density of 0.61 mA·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.

Keywords

P-doped carbon nanotubesnitrogen reduction reactionactive sitesreaction pathwayelectrocatalysis

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Nano Research
Volume 13 Issue 5,
May 2020
Pages 1376-1382
DOI: 10.1007/s12274-020-2637-8
Cite this article:
Yuan L-P, Wu Z-Y, Jiang W-J, et al. Phosphorus-doping activates carbon nanotubes for efficient electroreduction of nitrogen to ammonia. Nano Research, 2020, 13(5): 1376-1382. https://doi.org/10.1007/s12274-020-2637-8
Topics:
Cost effectivenessElectrocatalysis ElectrocatalystsElectrolytic reduction Energy efficiencyKinetic theoryNitrogenOrganic polymersPhosphorus

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Received: 25 September 2019
Revised: 31 December 2019
Accepted: 02 January 2020
Published: 15 January 2020
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020
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