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Light-Driven Trap Engineering in Direct Z-Scheme Channels for Ultrafast N2 Fixation.

Cun-Biao Lin1, De-Bo Lin1, Wen-Xian Chen1

  • 1H-PSI Computational Chemistry Lab, Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P.R. China.

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|December 8, 2025
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Summary
This summary is machine-generated.

Defect engineering in C7N6/MoSe2 heterojunctions creates shallow trap states. These states accelerate recombination, enhancing photocatalytic nitrogen fixation efficiency under ambient conditions.

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Area of Science:

  • Materials Science
  • Computational Chemistry
  • Catalysis

Background:

  • Efficient photocatalytic nitrogen fixation is crucial for sustainable ammonia production.
  • Understanding charge carrier dynamics in heterojunctions is key to optimizing photocatalyst performance.
  • Defect engineering offers a promising route to tune electronic properties of materials.

Purpose of the Study:

  • To investigate the role of Se vacancy and B atom doping in the C7N6/MoSe2 heterojunction for photocatalytic N2 fixation.
  • To elucidate the mechanisms of charge carrier transport, recombination, and N2 activation.
  • To enhance ammonia selectivity and efficiency under ambient conditions.

Main Methods:

  • Density Functional Theory (DFT) combined with Nonadiabatic Molecular Dynamics (NAMD).
  • Real-time Time-Dependent DFT (RT-TDDFT) for analyzing carrier dynamics.
  • Computational modeling of heterojunctions with defect strategies.

Main Results:

  • Shallow charge trap states induced by Se vacancy and B doping regulate carrier transport and velocity.
  • Rapid capture-release mechanism accelerates interlayer recombination, reducing carrier lifetime.
  • Photogenerated electrons activate N2 within 55 fs, facilitated by Boron dopants.
  • Achieved a low limiting potential of -0.23 V and improved NH3 selectivity.

Conclusions:

  • Defect engineering in C7N6/MoSe2 Z-scheme heterojunctions effectively modulates charge migration and recombination.
  • Shallow trap states enhance carrier redox capabilities, crucial for efficient photocatalytic N2 fixation.
  • This study provides a novel perspective for designing ambient photocatalysts for nitrogen fixation.