Periodic Defect Engineering of Iron–Nitrogen–Carbon Catalysts for Nitrate Electroreduction to Ammonia
Runxi Zhu, Yanyang Qin, Tiantian Wu, Shujiang Ding, Yaqiong Su
Abstract
Abstract Iron–nitrogen–carbon single atom catalyst (SAC) is regarded as one of the promising electrocatalysts for NO 3 − reduction reaction (NO 3 RR) to NH 3 due to its high activity and selectivity. However, synergistic effects of topological defects and FeN 4 active moiety in Fe–N–C SAC have rarely been investigated. By performing density functional theory (DFT) calculations, 13 defective graphene FeN 4 with 585, 484, and 5775 topological line defects are constructed, yielding 585‐68‐FeN 4 with optimal NO 3 RR catalytic activity, high selectivity, as well as robust anti‐dissolution stability. The high NO 3 RR activity on 585‐68‐FeN 4 is well explained by the high valence state of Fe center as well as asymmetric charge distribution on FeN 4 moiety influenced by 5‐ and 8‐member rings. This DFT work provides theoretical guidance for engineering NO 3 RR performance of iron–nitrogen–carbon catalysts by modulating periodic topological defects.