Unlocking the Nitrogen Reduction Electrocatalyst with a Dual-Metal-Boron System: From High-Throughput Screening to...

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Dual-metal catalysts offer abundant active sites and tunable properties.
• Metal borides are effective in splitting inert chemical bonds, like in N₂.
• Combining these systems creates novel dual-metal-boron catalysts.

Purpose of the Study:

• To investigate the performance of dual-metal-boron systems for the nitrogen reduction reaction (NRR).
• To explore 66 different dual-transition metal embedded in boron-doped graphene (BG) systems.
• To identify stable and efficient electrocatalysts for NRR.

Main Methods:

• First-principles simulations were used to examine 66 dual-transition metal@BG systems.
• Microkinetic modeling was employed to analyze reaction rates.
• Machine learning methods were utilized to understand catalytic mechanisms.

Main Results:

• Dual-TM@BG systems demonstrated excellent thermodynamic and electrochemical stability.
• Fe-Fe- and Fe-Co-doped BG showed superior NRR performance with low limiting potentials (-0.29 and -0.32 V).
• These catalysts inhibited the hydrogen evolution reaction and exhibited ultrafast NH₃ production rates.

Conclusions:

• Fe-Fe- and Fe-Co-doped BG are promising electrocatalysts for NRR.
• Dual-metal-boron systems are feasible for NRR applications.
• Catalyst performance correlates with the sum of the radii of the transition metal atoms.