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Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction

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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.

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Acknowledgments

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 (https://www.shiyanjia.com) for the XPS and liquid contact angle tests.

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Authors and Affiliations

  1. 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

    Lijuan Niu, Ziwen Liu, Guohua Liu, Xupeng Zong, Li An, Dan Qu, Xiayan Wang & Zaicheng Sun

  2. 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

    Mengxuan Li & Xiaoming Sun

  3. Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun, 130103, China

    Dandan Wang

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  1. Lijuan Niu
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  2. Ziwen Liu
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  3. Guohua Liu
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  4. Mengxuan Li
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  7. Li An
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  9. Xiaoming Sun
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  10. Xiayan Wang
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Correspondence to Li An or Zaicheng Sun.

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Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction

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Niu, L., Liu, Z., Liu, G. et al. Surface hydrophobic modification enhanced catalytic performance of electrochemical nitrogen reduction reaction. Nano Res. 15, 3886–3893 (2022). https://doi.org/10.1007/s12274-021-4015-6

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