Screening Janus-2H-WSSe with Adsorbed Transition Metals as Efficient Catalyst for Nitrogen Reduction Reaction

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Electrocatalytic nitrogen reduction reaction (NRR) is a key process for sustainable ammonia synthesis.
• Developing efficient electrocatalysts for NRR under ambient conditions remains a significant challenge.

Purpose of the Study:

• To investigate the structural stability and NRR catalytic activity of transition metal (TM) atoms adsorbed on Janus 2H-WSSe monolayers.
• To identify promising single-atom catalysts (SACs) for efficient nitrogen fixation.

Main Methods:

• First-principles calculations were employed to study 29 transition metals (Sc-Hg) on Janus 2H-WSSe.
• Screening of potential SACs based on limiting potential and Faradaic efficiency.
• Analysis of catalytic activity trends using descriptors like ΔG*NNH, ΔG*NH2, ΔG*N, and work function (φ).

Main Results:

• Six TM@WSSe systems (Os, Re, Ir, Mo) were identified as promising SACs with low limiting potentials (-0.36 to -0.73 V) and high Faradaic efficiency (>90.61%).
• High catalytic activity is attributed to d-orbital interactions between TM atoms and N2 molecules, facilitating N2 activation and hydrogenation.
• The TM@WSSe system with ΔG*N = -1.38 eV and φ = 6 exhibited optimal catalytic performance.

Conclusions:

• Janus 2H-WSSe monolayers decorated with specific transition metals are effective supports for single-atom catalysts in NRR.
• Tuning adsorption energy descriptors (ΔG*NH2 or ΔG*NNH) and work function is crucial for optimizing NRR activity.
• This study provides valuable insights for designing advanced electrocatalysts for nitrogen fixation.