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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Controlling molecular catalyst arrangement on electrodes is key for optimal electrocatalyst performance.
  • Molybdenum-sulfur (Mo-S) clusters show potential for hydrogen evolution reactions (HER) in generating carbon-free fuels.

Purpose of the Study:

  • To synthesize and characterize ordered arrangements of Mo-S molecular clusters using organic linkers.
  • To investigate the impact of organized Mo-S clusters on hydrogen evolution catalysis.

Main Methods:

  • Utilized organic linkers to create ordered dimers, cages, and chains of Mo-S clusters.
  • Determined structures using single-crystal X-ray diffraction.
  • Evaluated catalytic performance for hydrogen evolution.

Main Results:

  • Achieved a 40-fold enhancement in turnover frequency compared to unlinked clusters.
  • Demonstrated controlled periodic arrangement of clusters on electrodes (distance, orientation, density).
  • Developed Mo-S catalysts requiring only 89 mV overpotential for 10 mA cm-2 current density.

Conclusions:

  • Linkage via thiolate-Mo3S7 coordination bonds enables enhanced HER performance.
  • Ordered Mo-S clusters facilitate efficient hydrogen evolution at high catalyst loading.
  • This approach offers a superior alternative to existing Mo-S catalysts for electrocatalytic applications.