Enhanced Activity and Selectivity for Nitrogen Reduction Reaction in Electrides-Based Heterostructures: A DFT...

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Developing sustainable catalysts for ammonia synthesis is a key challenge.
• Two-dimensional heterostructures, especially single-atom catalysts (SACs), show promise.
• Electrides offer high surface activity and abundant free electrons for catalysis.

Purpose of the Study:

• To propose and investigate electride-graphene heterostructures (EGHS) as efficient catalysts for ammonia synthesis.
• To optimize charge distribution and catalytic performance using DFT calculations.
• To address challenges like excessive adsorbate binding in electride-based catalysts.

Main Methods:

• Density Functional Theory (DFT) calculations were employed.
• Electride-graphene heterostructures (EGHS) were modeled.
• Charge transfer and binding energies were analyzed to assess catalytic performance.

Main Results:

• Cr-doped EGHS (Cr@EGHS) demonstrated excellent performance for nitrogen reduction.
• A low limiting potential of -0.85 V and high selectivity were achieved.
• Modulating layer distance confirmed the role of charge transfer in N2 activation.

Conclusions:

• EGHS offer a novel strategy for designing efficient 2D heterostructure catalysts.
• Optimized charge transfer is crucial for enhancing catalytic activity in ammonia synthesis.
• These findings provide a reference for experimental synthesis of advanced catalysts.