电合成
法拉第效率
甲酰胺
甲醇
催化作用
化学
过电位
电解
电化学
阴极
电流密度
氨
无机化学
化学工程
材料科学
核化学
电极
有机化学
物理化学
工程类
物理
电解质
量子力学
作者
Jiang Shao,Nannan Meng,Yuting Wang,Baoshun Zhang,Kaiwen Yang,Cuibo Liu,Yifu Yu,Bin Zhang
标识
DOI:10.1002/anie.202213009
摘要
The scalable and durable electrosynthesis of high-valued organonitrogen compounds from carbon- and nitrogen-containing small molecules, especially operating at a high current density, is highly desirable. Here, a one-pot electrooxidation method to synthesize formamide (HCONH2 ) from methanol and ammonia over a commercial boron-doped diamond (BDD) catalyst is reported. The formamide selectivity from methanol and formamide Faradaic efficiency (FE HCONH2${{_{{\rm HCONH}{_{2}}}}}$ ) achieve 73.2 % and 41.2 % at the current density of 120 mA cm-2 with high durability. The C-N bond originates from the nucleophilic attack of ammonia on an aldehyde-like intermediate. Impressively, an 8 L electrolyzer is employed for the pilot plant test over a 2200 cm2 BDD electrode, which exhibits 33.5 % FE HCONH2${{_{{\rm HCONH}{_{2}}}}}$ at 120 mA cm-2 (current: 264 A) with a yield rate of 36.9 g h-1 , demonstrating the potential of this technique for large-scale electrosynthesis of formamide.
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