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Nano Research 2021, 14(11): 4093-4099 https://doi.org/10.1007/s12274-021-3348-5
Research Article | Issue | Published: 16 February 2021

Tuning the performance of nitrogen reduction reaction by balancing the reactivity of N2 and the desorption of NH3

Show Author's Information Lijuan Niu1,  Dandan Wang2,  Kang Xu3,  Weichang Hao3,  Li An1( ),  Zhenhui Kang4,5( ),  Zaicheng Sun1( )
Beijing Key Laboratory for Green Catalysis and Separation Center of Excellence for Environmental Safety and Biological Effects, Faculty of Environment and Life, Beijing University of TechnologyBeijing 100124 China
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education College of Physics, Jilin Normal UniversitySiping 136000 China
Department of Physics Key Laboratory of Micro-Nano Measurement, Manipulation and Physics, Ministry of Education, Beihang UniversityBeijing 100191 China
Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices Institute of Functional Nano and Soft Materials (FUNSOM), Soochow UniversitySuzhou 215123 China
Macao Institute of Materials Science and Engineering Macau University of Science and TechnologyMacau SAR Taipa 999078 China
Keywords:
MoS2, electrocatalyst, nitrogen reduction reaction, nitrogen-fixing
Topics:
AmmoniaCatalyst activityElectrocatalystsElectrolytic reduction Gas adsorptionIron compoundsLayered semiconductorsMolybdenum compoundsNitrogenVanadium compounds
Cite this article:
Niu L, Wang D, Xu K, et al. Tuning the performance of nitrogen reduction reaction by balancing the reactivity of N2 and the desorption of NH3. Nano Research, 2021, 14(11): 4093-4099. https://doi.org/10.1007/s12274-021-3348-5
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Abstract Full text Electronic supplementary material About this article

Electrochemical reduction of nitrogen to ammonia under mild conditions provides an intriguing approach for energy conversion. A grand challenge for electrochemical nitrogen reduction reaction (NRR) is to design a superior electrocatalyst to obtain high performance including high catalytic activity and selectivity. In the NRR process, the three most important steps are nitrogen adsorption, nitrogen activation, and ammonia desorption. We take MoS2 as the research object and obtain catalysts with different electronic densities of states through the doping of Fe and V, respectively. Using a combination of experiments and theoretical calculations, it is demonstrated that V-doped MoS2 (MoS2-V) shows better nitrogen adsorption and activation, while Fe-doped MoS2 (MoS2-Fe) obtains the highest ammonia yield in experiments (20.11 µg·h-1·mgcat–1.) due to its easier desorption of ammonia. Therefore, an appropriate balance between nitrogen adsorption, nitrogen activation, and ammonia desorption should be achieved to obtain highly efficient NRR electrocatalysts.


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About this article

Tuning the performance of nitrogen reduction reaction by balancing the reactivity of N2 and the desorption of NH3

Show Author's information Lijuan Niu1, Dandan Wang2, Kang Xu3, Weichang Hao3, Li An1( ), Zhenhui Kang4,5( ), Zaicheng Sun1( )
Beijing Key Laboratory for Green Catalysis and Separation Center of Excellence for Environmental Safety and Biological Effects, Faculty of Environment and Life, Beijing University of TechnologyBeijing 100124 China
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education College of Physics, Jilin Normal UniversitySiping 136000 China
Department of Physics Key Laboratory of Micro-Nano Measurement, Manipulation and Physics, Ministry of Education, Beihang UniversityBeijing 100191 China
Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices Institute of Functional Nano and Soft Materials (FUNSOM), Soochow UniversitySuzhou 215123 China
Macao Institute of Materials Science and Engineering Macau University of Science and TechnologyMacau SAR Taipa 999078 China

Abstract

Electrochemical reduction of nitrogen to ammonia under mild conditions provides an intriguing approach for energy conversion. A grand challenge for electrochemical nitrogen reduction reaction (NRR) is to design a superior electrocatalyst to obtain high performance including high catalytic activity and selectivity. In the NRR process, the three most important steps are nitrogen adsorption, nitrogen activation, and ammonia desorption. We take MoS2 as the research object and obtain catalysts with different electronic densities of states through the doping of Fe and V, respectively. Using a combination of experiments and theoretical calculations, it is demonstrated that V-doped MoS2 (MoS2-V) shows better nitrogen adsorption and activation, while Fe-doped MoS2 (MoS2-Fe) obtains the highest ammonia yield in experiments (20.11 µg·h-1·mgcat–1.) due to its easier desorption of ammonia. Therefore, an appropriate balance between nitrogen adsorption, nitrogen activation, and ammonia desorption should be achieved to obtain highly efficient NRR electrocatalysts.

Keywords: MoS2, electrocatalyst, nitrogen reduction reaction, nitrogen-fixing

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Publication history
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Acknowledgements

Publication history

Received: 21 November 2020
Revised: 28 December 2020
Accepted: 20 January 2021
Published: 16 February 2021
Issue date: November 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

This work was financially supported by the Beijing Municipal High Level Innovative Team Building Program (No. IDHT­20180504), Beijing Outstanding Young Scientists Program (No. BJJWZYJH01201910005017), the National Natural Science Foundation of China (Nos. 51801006, 21805004, 21671011, and 21872001), Beijing Natural Science Foundation (Nos. KZ201710005002 and 2192005), Beijing Municipal Science and Natural Science Fund Project (No. KM201910005016), China Postdoctoral Science Foundation (No. 2018M641133), Beijing Postdoctoral Research Foundation (No. 2018-ZZ-021) and Chaoyang District Postdoctoral Research Foundation (No. 2018-ZZ-026). These funding agencies are acknowledged.

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