Yuan-Zi Xu, Daniel F Abbott, Lok Nga Poon, Victor Mougel
{"title":"Two-step tandem electrochemical conversion of oxalic acid and nitrate to glycine.","authors":"Yuan-Zi Xu, Daniel F Abbott, Lok Nga Poon, Victor Mougel","doi":"10.1039/d5ey00016e","DOIUrl":null,"url":null,"abstract":"<p><p>This study presents a facile tandem strategy for improving the efficiency of glycine electrosynthesis from oxalic acid and nitrate. In this tandem electrocatalytic process, oxalic acid is first reduced to glyoxylic acid, while nitrate is reduced to hydroxylamine. Subsequent coupling of these two precursors results in the formation of a C-N bond, producing the intermediate glyoxylic acid oxime, which is further reduced <i>in situ</i> to glycine. Here we show, using only a simple Pb foil electrode, which maximizes the yield of the first step of the transformation (<i>i.e.</i> the reduction of oxalic acid to glyoxylic acid) prior to the coupling step allows for an unprecedented selectivity and conversion for glycine electrosynthesis to be achieved. Overall, a maximum glycine faradaic efficiency (FE) of 59% is achieved at -300 mA cm<sup>-2</sup> and a high glycine partial current density of -232 mA cm<sup>-2</sup> and a glycine production rate of 0.82 mmol h<sup>-1</sup> cm<sup>-2</sup> are attained at -400 mA cm<sup>-2</sup>, thereby paving the way for an energy and economically efficient electrochemical synthesis of glycine.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" ","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11973474/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"EES catalysis","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1039/d5ey00016e","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
Abstract
This study presents a facile tandem strategy for improving the efficiency of glycine electrosynthesis from oxalic acid and nitrate. In this tandem electrocatalytic process, oxalic acid is first reduced to glyoxylic acid, while nitrate is reduced to hydroxylamine. Subsequent coupling of these two precursors results in the formation of a C-N bond, producing the intermediate glyoxylic acid oxime, which is further reduced in situ to glycine. Here we show, using only a simple Pb foil electrode, which maximizes the yield of the first step of the transformation (i.e. the reduction of oxalic acid to glyoxylic acid) prior to the coupling step allows for an unprecedented selectivity and conversion for glycine electrosynthesis to be achieved. Overall, a maximum glycine faradaic efficiency (FE) of 59% is achieved at -300 mA cm-2 and a high glycine partial current density of -232 mA cm-2 and a glycine production rate of 0.82 mmol h-1 cm-2 are attained at -400 mA cm-2, thereby paving the way for an energy and economically efficient electrochemical synthesis of glycine.
本研究提出了一种提高草酸和硝酸盐电合成甘氨酸效率的简易串联策略。在串联电催化过程中,草酸首先被还原为乙醛酸,而硝酸盐被还原为羟胺。随后这两个前体的偶联导致C-N键的形成,产生中间的乙醛酸肟,它在原位进一步还原为甘氨酸。在这里,我们表明,仅使用一个简单的铅箔电极,最大限度地提高了在耦合步骤之前转化的第一步(即草酸还原为乙醛酸)的产量,从而实现了甘氨酸电合成的前所未有的选择性和转化。总体而言,在-300 mA cm-2条件下,甘氨酸的最大法拉第效率(FE)达到59%,在-400 mA cm-2条件下,甘氨酸的高偏电流密度达到-232 mA cm-2,甘氨酸的产率达到0.82 mmol h-1 cm-2,从而为高效节能的甘氨酸电化学合成铺平了道路。