Electricity-driven enzymatic dynamic kinetic oxidation

Beibei Zhao, Yuanyuan Xu, Qin Zhu, Aokun Liu, Xichao Peng, Tianying Zhang, Lu Yu, Yan Zhang and Xiaoqiang Huang ()
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Beibei Zhao: Nanjing University
Yuanyuan Xu: Nanjing University
Qin Zhu: Nanjing University
Aokun Liu: University of Science and Technology of China
Xichao Peng: Nanjing University
Tianying Zhang: Nanjing University
Lu Yu: University of Science and Technology of China
Yan Zhang: Nanjing University
Xiaoqiang Huang: Nanjing University

Nature, 2025, vol. 643, issue 8072, 699-704

Abstract: Abstract Electrochemistry is undergoing a resurgence in synthetic chemistry and has compelling advantages1. Repurposing natural enzymes through synthetic chemical strategies holds promise for exploring new chemical space2–6. Elegant strategies, including directed evolution7–10, artificial enzymes11 and photoenzymatic catalysis12,13, have demonstrated their capacities for expanding the applications of enzymes in both academia and industry. However, the integration of electrochemistry with enzymes has primarily been limited to replicating previously established enzyme functions14–16. Key challenges in achieving new enzyme reactivity with electricity include compatibility issues and difficulties in heterogeneous electron transfer. Here we report the reshaping of thiamine-dependent enzymes with ferrocene-mediated electrocatalysis to unlock an unnatural dynamic kinetic oxidation of α-branched aldehydes. This robust electroenzymatic approach yields various bioactive (S)-profens with up to 99% enantiomeric excess; it is applicable with whole cells overexpressing the enzyme and using down to 0.05 mol% enzyme loadings. Mechanistic investigations show multiple functions of the electroenzyme in precise substrate discrimination, accelerating racemization and facilitating kinetically matched electron transfer events.

Date: 2025
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DOI: 10.1038/s41586-025-09178-6

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