High-throughput screening for efficient dual-atom catalysts in electrocatalytic nitrate reduction to ammonia via dissociation-association mechanism

As a technology that can not only address water pollution but also generate ammonia, electrocatalytic reduction of nitrate (NO₃RR) to ammonia has seen a new upsurge in recent years. Herein, through first-principles high-throughput screening, we discovered that g-C₃N₄-based dual-atom catalysts (M1M2/g-C₃N₄, M1 = M2 = Ti, V, Cr, Mn, Fe, Co, Ni, Cu) exhibit extraordinary NO₃RR catalytic performance. The multilevel descriptor elucidates the origin of the NO₃RR reaction and facilitates rapid screening of candidate materials. The results indicate that TiFe/g-C₃N₄ possesses the best performance (U_L = − 0.21 eV) among the 36 M1M2/g-C₃N₄ catalysts evaluated. Impressively, TiFe/g-C₃N₄ dual-atom catalysts differ from single-atom catalysts in that they follow a distinct dissociation-association reaction mechanism. Further orbital analysis signifies that this behavior arises from the synergistic effect of dual-atom metals. By establishing the correlation between structure and performance, our predictions contribute to the advancement of NO₃RR as a method of ammonia production. This study holds promise for addressing water pollution while simultaneously harnessing renewable resources.