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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Electrocatalytic nitrogen reduction reaction (NRR) offers a sustainable alternative to the Haber-Bosch process for ammonia (NH3) production.
  • Developing efficient NRR catalysts and understanding their mechanisms are significant challenges.

Purpose of the Study:

  • To design and synthesize novel atomically dispersed tungsten (W) catalysts for enhanced NRR.
  • To investigate the relationship between charge transfer and NRR performance.
  • To elucidate the catalytic mechanism of W-based catalysts for ammonia synthesis.

Main Methods:

  • Atomically dispersed W atoms were embedded into V2-xCTz using a self-capture method.
  • Electrocatalytic performance was evaluated by measuring ammonia yield and Faradaic efficiency (FE).
  • Density Functional Theory (DFT) computations were employed to study reaction mechanisms and energy barriers.

Main Results:

  • The n-W/V2-xCTz catalyst achieved a record ammonia yield of 121.8 μg h-1 mg-1 and FE of 34.2% at -0.1 V vs RHE.
  • DFT calculations showed synergistic effects of neighboring W atoms, lowering the limiting potential (UL) to 0.32 V.
  • A linear relationship between UL and integrated-crystal orbital Hamilton population (ICOHP) was established as an activity descriptor.

Conclusions:

  • Atomically dispersed W catalysts exhibit exceptional performance for electrocatalytic NRR.
  • Neighboring single atoms play a crucial role in enhancing reaction kinetics through synergistic effects.
  • The study provides a new descriptor for NRR activity and insights into the underlying electronic structure-performance relationship.