Electrocatalytic Synthesis of Pyridine Oximes using in Situ Generated NH 2 OH from NO species on Nanofiber Membranes Derived from NH 2 ‐MIL‐53(Al)
作者:Runan Xiang, Shihan Wang, Peisen Liao, Fangyan Xie, Jiawei Kang, Suisheng Li, Jiahui Xian, Linna Guo, Guangqin Li · 发表于:Angewandte Chemie International Edition · 年份:2023 · DOI:10.1002/anie.202312239 · 被引用次数:100 · 研究领域:Ammonia Synthesis and Nitrogen Reduction、Nanomaterials for catalytic reactions、Metal-Organic Frameworks: Synthesis and Applications
Abstract Pyridine oximes produced from aldehyde or ketone with hydroxylamine (NH 2 OH) have been widely applied in pharmaceutics, enzymatic and sterilization. However, the important raw material NH 2 OH exhibits corrosive and unstable properties, leading to substantial energy consumption during storage and transportation. Herein, this work presents a novel method for directly synthesizing highly valuable pyridine oximes using in situ generated NH 2 OH from electrocatalytic NO reduction with well‐design nanofiber membranes (Al‐NFM) derived from NH 2 ‐MIL‐53(Al). Particularly, 2‐pyridinealdoxime, the precursor of antidote pralidoxime (2‐PAM) for nerve agents suffering from scarcity and high cost, was achieved with a Faraday efficiency up to 49.8 % and a yield of 92.1 %, attributing to the high selectivity of NH 2 OH production on Al‐NFM, further easily reacted with iodomethane to produce 2‐PAM. This study proposes a creative approach, having wide universality for synthesizing pyridine and other oximes with a range of functional groups, which not only facilitates the conversion of exhaust gas (NO) and waste water (NO 2 − ) into valuable chemicals especially NH 2 OH production and in situ utilization through electrochemistry, but also holds significant potential for synthesis of neuro detoxifying drugs to humanity security.