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Nano Research 2019, 12(5): 1181-1186 https://doi.org/10.1007/s12274-019-2378-8
Research Article | Issue | Published: 29 March 2019

gt-C3N4 coordinated single atom as an efficient electrocatalyst for nitrogen reduction reaction

Show Author's Information Lifu Zhang1,2,  Wanghui Zhao2,  Wenhua Zhang2( ),  Jing Chen1,3,  Zhenpeng Hu1( )
School of Physics,Nankai University,Tianjin,300071,China;
Hefei National Laboratory for Physical Sciences at the Microscale,CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information & Quantum Physics, University of Science and Technology of China,Hefei,230026,China;
Collaborative Innovation Center of Extreme Optics,Shanxi University,Taiyuan,030006,China;
Keywords:
single-atom catalyst, first-principles calculation, nitrogen reduction reaction, Gibbs free energy
Topics:
CalculationsCoordination reactionsElectrocatalystsElectrolytic reduction Free energy NitrogenPrecious metals
Cite this article:
Zhang L, Zhao W, Zhang W, et al. gt-C3N4 coordinated single atom as an efficient electrocatalyst for nitrogen reduction reaction. Nano Research, 2019, 12(5): 1181-1186. https://doi.org/10.1007/s12274-019-2378-8
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Abstract Full text Electronic supplementary material About this article

The electrochemical reduction of nitrogen to ammonia is a promising way to produce ammonia at mild condition. The design and preparation of an efficient catalyst with high ammonia selectivity is critical for the real applications. In this work, a series of transition metal (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, and Cd) atoms supported by gt-C3N4 (TM/gt-C3N4) are investigated as electrocatalysts for the nitrogen reduction reaction (NRR) based on density functional calculations. It is found that Mo/gt-C3N4 with a limiting potential of -0.82 V is the best catalyst for standing-on adsorbed N2 cases. While for lying-on adsorbed N2 cases, V/gt-C3N4 with a limiting potential of -0.79 V is better than other materials. It is believed that this work provides several promising candidates for the non-noble metal electrocatalysts for NRR at mild condition.


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Electronic supplementary material
About this article

gt-C3N4 coordinated single atom as an efficient electrocatalyst for nitrogen reduction reaction

Show Author's information Lifu Zhang1,2, Wanghui Zhao2, Wenhua Zhang2( ), Jing Chen1,3, Zhenpeng Hu1( )
School of Physics,Nankai University,Tianjin,300071,China;
Hefei National Laboratory for Physical Sciences at the Microscale,CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information & Quantum Physics, University of Science and Technology of China,Hefei,230026,China;
Collaborative Innovation Center of Extreme Optics,Shanxi University,Taiyuan,030006,China;

Abstract

The electrochemical reduction of nitrogen to ammonia is a promising way to produce ammonia at mild condition. The design and preparation of an efficient catalyst with high ammonia selectivity is critical for the real applications. In this work, a series of transition metal (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, and Cd) atoms supported by gt-C3N4 (TM/gt-C3N4) are investigated as electrocatalysts for the nitrogen reduction reaction (NRR) based on density functional calculations. It is found that Mo/gt-C3N4 with a limiting potential of -0.82 V is the best catalyst for standing-on adsorbed N2 cases. While for lying-on adsorbed N2 cases, V/gt-C3N4 with a limiting potential of -0.79 V is better than other materials. It is believed that this work provides several promising candidates for the non-noble metal electrocatalysts for NRR at mild condition.

Keywords: single-atom catalyst, first-principles calculation, nitrogen reduction reaction, Gibbs free energy

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Publication history
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Acknowledgements

Publication history

Received: 20 December 2018
Revised: 22 February 2019
Accepted: 12 March 2019
Published: 29 March 2019
Issue date: May 2019

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21773124 and 21473167), the Fundamental Research Funds for the Central Universities (No. WK3430000005), the Fok Ying Tung Education Foundation (No. 151008), and partially by the support of China Scholarship Council (CSC) (File No. 201706345015). The calculations were performed on the super-computing system in USTC-SCC, Tianjin-SCC and Guangzhou-SCC.

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