Li Peifeng, Wang Kaixuan, Zhang Biaobiao
Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science and Research Center for Industries of the Future, Westlake University, Hangzhou 310024, Zhejiang, China.
Institute of Natural Sciences, Westlake Institute for Advanced Study, Hangzhou 310024, Zhejiang, China.
ACS Appl Mater Interfaces. 2024 Oct 23;16(42):57171-57179. doi: 10.1021/acsami.4c12925. Epub 2024 Oct 10.
Electrosynthesis is a rising and attractive method for efficient amino acid production. However, industrial-grade electrosynthesis of high-value amino acids from simple carbon and nitrogen substrates is confronted with a great challenge. Herein, we design a dual-site PbBi alloy catalyst for various amino acids' electrosynthesis from keto acids and nitrate. An alanine Faradaic efficiency of 59.7% is delivered at -1.5 V vs SCE, reaching the industrial current density of 570 mA cm with high catalytic durability of the porous PbBi catalyst. In the tandem reaction process, nitrate is first converted to NHOH via electrochemical reduction mainly over the Bi site. Then the obtained NHOH integrates with the α-keto acid to form the oxime intermediate. Lastly, the Pb site facilitates the electroreduction of oxime to the final amino acids. More importantly, over 10 kinds of α-amino acids can be successfully synthesized in excellent FE and high yield at high current density, indicating the superior catalytic activity and wide universality of our strategy. In short, this work opens up a novel approach to realize the one-pot electrosynthesis of various amino acids from renewable biomass feedstocks and nitrate waste industrially.
电合成是一种新兴且有吸引力的高效生产氨基酸的方法。然而,从简单的碳源和氮源底物进行工业级电合成高价值氨基酸面临着巨大挑战。在此,我们设计了一种双位点PbBi合金催化剂,用于从酮酸和硝酸盐电合成各种氨基酸。在相对于标准甘汞电极(SCE)为 -1.5 V的电位下,丙氨酸的法拉第效率达到59.7%,多孔PbBi催化剂在570 mA cm²的工业电流密度下具有高催化耐久性。在串联反应过程中,硝酸盐首先主要通过在Bi位点上的电化学还原转化为NHOH。然后所得的NHOH与α-酮酸结合形成肟中间体。最后,Pb位点促进肟电还原为最终的氨基酸。更重要的是,超过10种α-氨基酸能够在高电流密度下以优异的法拉第效率和高产率成功合成,这表明我们的策略具有卓越的催化活性和广泛的通用性。简而言之,这项工作开辟了一种新方法,可在工业上实现从可再生生物质原料和硝酸盐废料一锅法电合成各种氨基酸。