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Nano Research 2022, 15(5): 3886-3893 https://doi.org/10.1007/s12274-021-4015-6
Research Article | Issue | Published: 07 January 2022

Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction

Show Author's Information Lijuan Niu1,  Ziwen Liu1,  Guohua Liu1,  Mengxuan Li2,  Xupeng Zong1,  Dandan Wang3,  Li An1( ),  Dan Qu1,  Xiaoming Sun2,  Xiayan Wang1,  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 Technology, Beijing 100124, China
State Key Laboratory of Chemical Resource Engineering College of Energy, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun 130103, China
Keywords:
density functional theory calculations, nitrogen reduction reaction, MoS2 electrocatalyst , hydrophobic modification
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Cite this article:
Niu L, Liu Z, Liu G, et al. Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction. Nano Research, 2022, 15(5): 3886-3893. https://doi.org/10.1007/s12274-021-4015-6
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Abstract Full text Electronic supplementary material About this article

Electrocatalytic nitrogen reduction reaction (NRR) is a sustainable approach for NH3 production with low energy consumption. However, competing hydrogen reduction reaction (HER) in aqueous solution results in low NH3 production and Faraday efficiency (FE). Here, MoS2 nanostructures with a hydrophobic surface are synthesized by alkyl thiols modification. Aerophilic and hydrophobic surface facilitates an efficient three-phase contact of N2, H2O, and catalyst. Thus, localized concentrated N2 molecules can overcome the mass transfer limitation of N2 and depress the HER due to lowering the proton contacts. Although the active-sites decrease with the increase of the alkyl chain since the thiol may cover the active site, the optimized electrocatalyst achieves NH3 yield of 12.86 × 10−11 mol·cm−2·s−1 at −0.25 V and 22.23% FE, which are 4.3 and 24 times higher than those of MoS2-CP electrocatalyst, respectively. The increased catalytic performance is attributed to the high N2 adsorption and depressed HER.


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Abstract
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Electronic supplementary material
About this article

Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction

Show Author's information Lijuan Niu1, Ziwen Liu1, Guohua Liu1, Mengxuan Li2, Xupeng Zong1, Dandan Wang3, Li An1( ), Dan Qu1, Xiaoming Sun2, Xiayan Wang1, 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 Technology, Beijing 100124, China
State Key Laboratory of Chemical Resource Engineering College of Energy, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun 130103, China

Abstract

Electrocatalytic nitrogen reduction reaction (NRR) is a sustainable approach for NH3 production with low energy consumption. However, competing hydrogen reduction reaction (HER) in aqueous solution results in low NH3 production and Faraday efficiency (FE). Here, MoS2 nanostructures with a hydrophobic surface are synthesized by alkyl thiols modification. Aerophilic and hydrophobic surface facilitates an efficient three-phase contact of N2, H2O, and catalyst. Thus, localized concentrated N2 molecules can overcome the mass transfer limitation of N2 and depress the HER due to lowering the proton contacts. Although the active-sites decrease with the increase of the alkyl chain since the thiol may cover the active site, the optimized electrocatalyst achieves NH3 yield of 12.86 × 10−11 mol·cm−2·s−1 at −0.25 V and 22.23% FE, which are 4.3 and 24 times higher than those of MoS2-CP electrocatalyst, respectively. The increased catalytic performance is attributed to the high N2 adsorption and depressed HER.

Keywords: density functional theory calculations, nitrogen reduction reaction, MoS2 electrocatalyst , hydrophobic modification

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Publication history
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Acknowledgements

Publication history

Received: 09 September 2021
Revised: 04 November 2021
Accepted: 23 November 2021
Published: 07 January 2022
Issue date: May 2022

Copyright

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

Acknowledgements

We acknowledge financial support from the Beijing Municipal High Level Innovative Team Building Program (No. IDHT20180504), Beijing Outstanding Young Scientist Program (No. BJJWZYJH01201910005017), the National Natural Science Foundation of China (Nos. 51801006, 21805004, 21872001, and 21936001), Beijing Natural Science Foundation (No. 2192005), and Beijing Municipal Science and Natural Science Fund Project (Nos. KM201910005016 and 2017000020124G085). The authors would like to thank the Shiyanjia Lab (www.shiyanjia.com) for the XPS and liquid contact angle tests.

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