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Highly Efficient Electrosynthesis of Glycine over an Atomically Dispersed Iron Catalyst
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2024-03-26 , DOI: 10.1021/jacs.4c01093
Yingying Cheng 1 , Shiqiang Liu 1 , Jiapeng Jiao 2 , Meng Zhou 1 , Yiyong Wang 1, 3 , Xueqing Xing 4 , Zhongjun Chen 4 , Xiaofu Sun 1, 3 , Qinggong Zhu 1, 3 , Qingli Qian 1, 3 , Congyang Wang 1, 3 , Huizhen Liu 1, 3 , Zhimin Liu 1, 3 , Xinchen Kang 1, 3 , Buxing Han 1, 2, 3
Affiliation  

Glycine is a nonessential amino acid that plays a vital role in various biological activities. However, the conventional synthesis of glycine requires sophisticated procedures or toxic feedstocks. Herein, we report an electrochemical pathway for glycine synthesis via the reductive coupling of oxalic acid and nitrate or nitrogen oxides over atomically dispersed Fe–N–C catalysts. A glycine selectivity of 70.7% is achieved over Fe–N–C-700 at −1.0 V versus RHE. Synergy between the FeN3C structure and pyrrolic nitrogen in Fe–N–C-700 facilitates the reduction of oxalic acid to glyoxylic acid, which is crucial for producing glyoxylic acid oxime and glycine, and the FeN3C structure could reduce the energy barrier of *HOOCCH2NH2 intermediate formation thus accelerating the glyoxylic acid oxime conversion to glycine. This new synthesis approach for value-added chemicals using simple carbon and nitrogen sources could provide sustainable routes for organonitrogen compound production.

中文翻译:

在原子分散的铁催化剂上高效电合成甘氨酸

甘氨酸是一种非必需氨基酸,在各种生物活动中发挥着至关重要的作用。然而,甘氨酸的常规合成需要复杂的程序或有毒的原料。在此,我们报道了通过草酸和硝酸盐或氮氧化物在原子分散的 Fe-N-C 催化剂上的还原偶联合成甘氨酸的电化学途径。在 -1.0 V(相对于 RHE)条件下,Fe-N-C-700 的甘氨酸选择性达到 70.7%。 Fe-N-C-700中的FeN 3 C结构与吡咯氮之间的协同作用有助于将草酸还原为乙醛酸,这对于生产乙醛酸肟和甘氨酸至关重要,并且FeN 3 C结构可以降低能垒*HOOCCH 2 NH 2中间体形成,从而加速乙醛酸肟转化为甘氨酸。这种使用简单碳源和氮源的增值化学品的新合成方法可以为有机氮化合物的生产提供可持续的途径。
更新日期:2024-03-26
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