Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Atomically Dispersed Sn Protuberance

作者：Zhang, Lijuan; Zhou, Hanfeng; Yang, Xiaoju; Zhang, Shengbo; Zhang, Haimin; Yang, Xuan; Su, Xintai; Zhang, Jiangwei^*; Lin, Zhang^*

来源：Angewandte Chemie - International Edition, 2023, 62(13).

DOI：10.1002/anie.202217473

• Atomically Dispersed Sn
• Hydrogen Evolution Suppression
• Main-Group Elements (MGEs)
• N-2 Reduction Reaction
• p-Electron Backdonation

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 NH3 yield (R-NH3) of 28.3 mu g h(-1) mg(cat)(-1) (7447 mu g h(-1) mg(Sn)(-1)) at -0.3 V. Furthermore, the enhanced N2Hx 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.

• 单位
  中国科学院; 华中科技大学