School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006, P. R. China.
SCNU Environmental Research Institute, Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety & MOE Key Laboratory of Theoretical Chemistry of Environment, South China Normal University, Guangzhou, 510006, China.
Angew Chem Int Ed Engl. 2023 Mar 20;62(13):e202217473. doi: 10.1002/anie.202217473. Epub 2023 Feb 20.
Atomically dispersed metal catalysts show potential advantages in N 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 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 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 yield (R ) of 28.3 μg h mg (7447 μg h mg ) at -0.3 V. Furthermore, the enhanced N H 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 fixation.
原子分散的金属催化剂由于其优异的活性和高效的金属利用，在氮还原反应 (NRR) 中显示出潜在的优势。不幸的是，由于其对 N 的吸附和活化能力差，报道的催化剂通常表现出不尽如人意的 NRR 活性。在此，我们通过与基底 C 和 O 的配位报告了一种新型的 Sn 原子分散的突起物 (ADP)，以诱导 Sn 位上的正电荷积累，从而提高其对 N 的吸附、活化和 NRR 性能。扩展 X 射线吸收精细结构 (EXAFS) 光谱证实了 Sn ADP 的局部配位结构。通过 Sn ADPs，NRR 活性显著提高，在-0.3 V 时表现出显著的 NH 产率 (R )为 28.3 μg h mg (7447 μg h mg )。此外，通过原位实验验证了增强的 N H 中间体，与 DFT 计算结果一致。这项工作为调节氮固定的活性和选择性开辟了一条新途径。
