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木质素衍生的碳纳米片促进丙酮酸电化学还原胺化生成丙氨酸。

Lignin-derived carbon nanosheets boost electrochemical reductive amination of pyruvate to alanine.

作者信息

Jia Shunhan, Tan Xingxing, Wu Limin, Zhao Ziwei, Song Xinning, Feng Jiaqi, Zhang Libing, Ma Xiaodong, Zhang Zhanrong, Sun Xiaofu, Han Buxing

机构信息

Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.

出版信息

iScience. 2023 Aug 29;26(10):107776. doi: 10.1016/j.isci.2023.107776. eCollection 2023 Oct 20.

Abstract

Efficient and sustainable amino acid synthesis is essential for industrial applications. Electrocatalytic reductive amination has emerged as a promising method, but challenges such as undesired side reactions and low efficiency persist. Herein, we demonstrated a lignin-derived catalyst for alanine synthesis. Carbon nanosheets (CNSs) were synthesized from lignin via a template-assisted method and doped with nitrogen and sulfur to boost reductive amination and suppress side reactions. The resulting N,S-co-doped carbon nanosheets (NS-CNSs) exhibited outstanding electrochemical performance. It achieved a maximum alanine Faradaic efficiency of 79.5%, and a yield exceeding 1,199 μmol h cm on NS-CNS, with a selectivity above 99.9%. NS-CNS showed excellent durability during long-term electrolysis. Kinetic studies including control experiments and theoretical calculations provided further insights into the reaction pathway. Moreover, NS-CNS catalysts demonstrated potential in upgrading real-world polylactic acid plastic waste, yielding value-added alanine with a selectivity over 75%.

摘要

高效且可持续的氨基酸合成对于工业应用至关重要。电催化还原胺化已成为一种有前景的方法,但诸如不期望的副反应和低效率等挑战仍然存在。在此,我们展示了一种用于丙氨酸合成的木质素衍生催化剂。通过模板辅助法从木质素合成了碳纳米片(CNSs),并掺杂氮和硫以促进还原胺化并抑制副反应。所得的氮、硫共掺杂碳纳米片(NS-CNSs)表现出出色的电化学性能。它在NS-CNS上实现了79.5%的最大丙氨酸法拉第效率,产率超过1199 μmol h cm,选择性高于99.9%。NS-CNS在长期电解过程中表现出优异的耐久性。包括对照实验和理论计算在内的动力学研究为反应途径提供了进一步的见解。此外,NS-CNS催化剂在升级实际的聚乳酸塑料废料方面显示出潜力,以超过75%的选择性产生增值丙氨酸。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c82/10502407/a7e169b602fe/fx1.jpg

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