Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia
Xuewan Wang, Dan Wu, Suyun Liu, Jiujun Zhang, Xian‐Zhu Fu, Jing‐Li Luo
Abstract
Abstract Efficient and robust single-atom catalysts (SACs) based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia (NRR) under ambient conditions. Herein, for the first time, a Mn–N–C SAC consisting of isolated manganese atomic sites on ultrathin carbon nanosheets is developed via a template-free folic acid self-assembly strategy. The spontaneous molecular partial dissociation enables a facile fabrication process without being plagued by metal atom aggregation. Thanks to well-exposed atomic Mn active sites anchored on two-dimensional conductive carbon matrix, the catalyst exhibits excellent activity for NRR with high activity and selectivity, achieving a high Faradaic efficiency of 32.02% for ammonia synthesis at − 0.45 V versus reversible hydrogen electrode. Density functional theory calculations unveil the crucial role of atomic Mn sites in promoting N 2 adsorption, activation and selective reduction to NH 3 by the distal mechanism. This work provides a simple synthesis process for Mn–N–C SAC and a good platform for understanding the structure-activity relationship of atomic Mn sites. Graphic Abstract