Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Atomically Dispersed Sn Protuberance.
Lijuan ZhangHanfeng ZhouXiaoju YangShengbo ZhangHaimin ZhangXuan YangXintai SuJiangwei ZhangZhang LinPublished in: Angewandte Chemie (International ed. in English) (2023)
Atomically dispersed metal catalysts show potential advantages in N 2 reduction reaction (NRR) due to their excellent activity and efficient metal utilization. Unfortunately, the reported catalysts usually exhibit unsatisfactory NRR activity due to their poor N 2 adsorption and activation. Herein, we report a novel Sn atomically dispersed protuberance (ADP) by coordination with substrate C and O to induce positive charge accumulation on Sn site for improving its N 2 adsorption, activation and NRR performance. The extended X-ray absorption fine structure (EXAFS) spectra confirmed the local coordination structure of the Sn ADPs. NRR activity was significantly promoted via Sn ADPs, exhibiting a remarkable NH 3 yield (R NH3 ) of 28.3 μg h -1 mg cat -1 (7447 μg h -1 mg Sn -1 ) at -0.3 V. Furthermore, the enhanced N 2 H x intermediates was verified by in situ experiments, yielding consistent results with DFT calculation. This work opens a new avenue to regulate the activity and selectivity of N 2 fixation.