Citation: Shuhong Wu, Meng Zhang, Shengmei Huang, Lihai Cai, Dannong He, Yitao Liu. Vacancy-enhanced Mo-N₂ interaction in MoSe₂ nanosheets enables efficient electrocatalytic NH₃ synthesis[J]. Chinese Chemical Letters, ;2023, 34(1): 107282. doi: 10.1016/j.cclet.2022.03.005 shu

Vacancy-enhanced Mo-N₂ interaction in MoSe₂ nanosheets enables efficient electrocatalytic NH₃ synthesis

Shuhong Wu ^{a, b} ,
Meng Zhang ^c ,
Shengmei Huang ^c ,
Lihai Cai ^{d, *,} ,
Dannong He ^a ,
Yitao Liu ^{b, c, *,}

a.
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
b.
National Engineering Research Center for Nanotechnology, Shanghai 200240, China
c.
Innovation Center for Textile Science and Technology, Donghua University, Shanghai 200051, China
d.
Institute of Systems Engineering, Academy of Military Sciences, Beijing 102300, China

lihai96@163.com

liu-yt03@dhu.edu.cn

Received Date: 12 October 2021
Revised Date: 7 January 2022
Accepted Date: 1 March 2022
Available Online: 4 March 2022

Figures(4)

NH₃ plays an essential role in human life since it is an important raw material for fertilizers, plastics and rubbers production. As an NH₃ synthesis technology under ambient conditions, electrocatalytic N₂ reduction reaction (NRR) has great potential to replace the energy-intensive Haber-Bosch process. The key of electrocatalytic NRR is the exploration of efficient catalysts. Transition metal Mo is promising since it exists naturally in nitrogenase due to the unique Mo-N₂ interaction; particularly in the form of 2D material such as MoSe₂, the surface area is maximized for more active sites. However, the NRR performance of MoSe₂ is still unsatisfactory because Mo is only exposed at the semi-open edge, and the electronegative Se-mantled surface area remains inaccessible to N₂. Herein, we propose a simple and effective strategy to create high-concentration Se vacancies in MoSe₂ through heteroatom doping induced lattice strain, which effectively enhances the Mo-N₂ interaction on the surface area. In result, high NH₃ yield (3.04 × 10^–10 mol s^–1 cm^–2) and Faraday efficiency (21.61%) are attained at –0.45 V vs. RHE in 0.1 mol/L Na₂SO₄.
- MoSe₂ nanosheets,
- Doping,
- Se vacancies,
- Mo–N₂ interaction,
- Electrocatalysis,
- NH₃ synthesis
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Vacancy-enhanced Mo-N₂ interaction in MoSe₂ nanosheets enables efficient electrocatalytic NH₃ synthesis