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Defect Engineering in MoSe2 for the Hydrogen Evolution Reaction: From Point Defects to Edges.

Haibo Shu1, Dong Zhou, Feng Li

  • 1National Laboratory for Infrared Physics, Shanghai Institute of Technical Physics, Chinese Academy of Science , 200083 Shanghai, China.

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|November 21, 2017
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Summary

Molybdenum diselenide (MoSe2) exhibits superior catalytic activity for the hydrogen evolution reaction (HER) compared to molybdenum disulfide (MoS2). This study reveals MoSe2

Keywords:
defectdensity functional theoryedgehydrogen evolution reactiontransition-metal dichalcogenides

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Area of Science:

  • Materials Science
  • Catalysis
  • Computational Chemistry

Background:

  • Developing inexpensive electrocatalysts for the hydrogen evolution reaction (HER) is vital for large-scale hydrogen production.
  • Two-dimensional molybdenum diselenide (MoSe2) shows promise as a nonprecious catalyst, but optimizing its active sites is key.
  • Active sites in MoSe2 catalysts are located at both the edges and the basal plane.

Purpose of the Study:

  • To investigate the structural stability, electrocatalytic activity, and HER mechanisms of various MoSe2 structures.
  • To explore the impact of point defects and edges on MoSe2's catalytic performance.
  • To propose a model correlating electronic structure with HER activity.

Main Methods:

  • First-principles calculations were employed to study MoSe2 catalytic structures.
  • Thermodynamic stability of defects and edges was assessed.
  • A Fermi-abundance model was developed to explain activity trends.

Main Results:

  • Thermodynamically stable defects and edges in MoSe2 exhibit higher HER activity than their MoS2 counterparts.
  • The Fermi-abundance model successfully correlates electronic structure with HER activity for MoSe2, MoS2, and Pt.
  • Two distinct HER mechanisms were identified: Volmer-Tafel and Volmer-Heyrovsky, depending on the MoSe2 structure.

Conclusions:

  • MoSe2 with optimized defects and edges demonstrates competitive HER activity compared to platinum-based catalysts.
  • The findings provide insights into designing highly active electrocatalysts for HER.
  • The proposed Fermi-abundance model offers a versatile tool for catalyst assessment.