Computational Insight into Defective Boron Nitride Supported Double-Atom Catalysts for Electrochemical Nitrogen Reduction

Abstract

Designing highly selective and efficient double-atom electrocatalysts (DACs) is essential for achieving a superior nitrogen-reduction reaction (NRR) performance. Herein, we explored the defective boron nitride–supported cage-like double-atom catalysts to rummage the qualified NRR catalysts. Based on a systematic evaluation of the stability, N2 adsorption, NRR selectivity and activity of 10 DACs of TM1-TM2@VB-BN, we predicted Ru-Ti@VB-BN to be the NRR candidate with a limiting potential of −0.40 V. Compared to the corresponding single-atom catalysts, the introduction of Ti/Mo modulates the d-band center of the active metal atom, which improves the NRR performance. Moreover, the magnetic Ru-Ti dimer can facilitate the transfer of charge to molecular N2, ensuring a significant activation of the inert N≡N bond. This research not only opens up new avenues for designing boron nitride–supported DACs for NRR, but also deepens the understanding of DACs in N2 activation.