Efficient electrosynthesis of alanine from α-keto acids over a self-supported electrocatalyst with superior activity†

IF 6.1 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Min Xu, Shengbo Zhang, Jiafang Liu, Hui Xu, Yong Jiang, Yunxia Zhang, Guozhong Wang and Haimin Zhang
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Abstract

Currently, electrocatalytic reductive amination of α-keto acids can achieve efficient, sustainable, and environmentally friendly production of amino acids under environmental conditions and developing efficient electrocatalysts is crucial for electrochemical amino acid synthesis. Herein, we have realized the one-step electrosynthesis of alanine using biomass-derived pyruvic acid (PA) and NH2OH as raw reactants in Na2SO4 electrolyte over a self-supported Cu/Ti electrode. The Cu/Ti self-supported electrode exhibited excellent electrocatalytic performance with a high alanine yield of 324 μmol and a favorable Faraday efficiency (FE) of 90.5% at −0.62 V (vs. RHE). In situ X-ray absorption spectroscopy (XAS) analyses indicated electron transfer from the Ti substrate to deposited Cu sites, and the resulting electron-rich Cu sites are favourable for the adsorption of intermediates and inhibit the competitive reaction of the hydrogen evolution reaction (HER), enhancing the alanine selectivity. Further in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) verified the reaction path during the electrochemical amino acid synthesis. Moreover, over 10 kinds of amino acids have been successfully electro-synthesized. Except for alanine, the obtained FEs of over six amino acids are 64.8–74.1%. This strategy presents a sustainable and green way for amino acid synthesis under ambient conditions using renewable energy.

Abstract Image

α-酮酸在自持型电催化剂上高效电合成丙氨酸
目前,α-酮酸电催化还原胺化可以实现在环境条件下高效、可持续、环保地生产氨基酸,开发高效的电催化剂是电化学合成氨基酸的关键。本文以生物质丙酮酸(PA)和NH2OH为原料,在Na2SO4电解液中,通过自支撑型Cu/Ti电极,实现了丙氨酸的一步电合成。Cu/Ti自支撑电极具有优异的电催化性能,在−0.62 V(相对于RHE)下,丙氨酸产率高达324 μmol,法拉第效率(FE)为90.5%。原位x射线吸收光谱(XAS)分析表明,电子从Ti基体转移到沉积Cu位点,生成富电子的Cu位点有利于中间体的吸附,抑制析氢反应(HER)的竞争反应,提高丙氨酸的选择性。进一步的原位衰减全反射表面增强红外吸附光谱(ATR-SEIRAS)验证了电化学氨基酸合成过程中的反应路径。此外,已经成功地电合成了10多种氨基酸。除丙氨酸外,其余6种氨基酸的FEs为64.8 ~ 74.1%。这一策略为利用可再生能源在环境条件下合成氨基酸开辟了一条可持续和绿色的道路。
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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