TY - JOUR AU - Wang, Xuewan AU - Wu, Dan AU - Liu, Suyun AU - Zhang, Jiujun AU - Fu, Xian‑Zhu AU - Luo, Jing‑Li PY - 2021/05/12 Y2 - 2024/03/28 TI - Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia JF - Nano-Micro Letters JA - Nano-Micro Lett VL - 13 IS - SE - Articles DO - 10.1007/s40820-021-00651-1 UR - https://nmlett.org/index.php/nml/article/view/891 SP - 125 AB - <p>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&nbsp;V versus reversible hydrogen electrode. Density functional theory calculations unveil the crucial role of atomic Mn sites in promoting N<sub>2</sub> adsorption, activation and selective reduction to NH<sub>3</sub> 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.</p><p>Highlights:</p><p>1 A manganese single-atom catalyst is developed via a facile folic acid self-assembly strategy.<br>2 The catalyst exhibits outstanding activity and selectivity for electrochemical reduction of nitrogen to ammonia (NRR).<br>3 Electrocatalytic mechanism of Mn–N<sub>3</sub> site for NRR is unveiled by a combination of experimental and computational study.</p> ER -