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Research Article

Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction

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
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Graphical Abstract

MoS2 after thiol modification increased the local N2 concentration, inhibited the hydrogen reduction reaction (HER), and facilitated the adsorption of N2, which further improved the nitrogen reduction reaction (NRR) activity.

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

nitrogen reduction reactionMoS2 electrocatalyst hydrophobic modificationdensity functional theory calculations

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Nano Research
Volume 15 Issue 5,
May 2022
Pages 3886-3893
DOI: 10.1007/s12274-021-4015-6
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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Received: 09 September 2021
Revised: 04 November 2021
Accepted: 23 November 2021
Published: 07 January 2022
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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