电合成
氟
中心(范畴论)
甲酰胺
阳极
化学
电化学
结晶学
物理化学
有机化学
电极
作者
Fan Dong,Shiyong Mou,Siyuan Liu,Weidong Dai,Yanjuan Sun
出处
期刊:Research Square - Research Square
日期:2024-03-18
标识
DOI:10.21203/rs.3.rs-4079378/v1
摘要
Abstract Anodic oxidative amidation (EOA) strategies offer a sustainable and potentially promising route for amide synthesis. However, the efficiency and activity of catalysts under oxidative conditions are highly dependent on noble metals. Herein, we present our experimental findings and fundamental understanding that fluorine-doped Nb 2 O 5 nanosheet arrays on carbon fiber (F-Nb 2 O 5 /CP) serve as an efficient and robust non-noble catalyst for the electrochemical synthesis of formamide from ammonia and methanol under ambient conditions. In 0.5 M KHCO 3 solution, this catalyst achieved a high Faradaic efficiency of 52.0%, with an N selectivity of 79.1% at 1.5 V versus Hg/HgO electrode. The catalyst exhibited remarkable stability, maintaining its performance over 120 h. By integrating in-situ spectroscopy studies with density functional theory calculations, we revealed that fluorine doping induces a shift in the d-band center of the Nb site. This shift alters the adsorption behavior of OH - and * NH 2 intermediate on the F-Nb 2 O 5 (100) surface, thereby effectively lowering the C-N coupling energy barrier, and boosting the production of formamide.
科研通智能强力驱动
Strongly Powered by AbleSci AI