Efficient bioelectrocatalytic NADH regeneration with a novel amino-functionalized viologen redox polymer

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry Pub Date : 2024-11-19 DOI:10.1016/j.bioelechem.2024.108850

Kavita Jayakumar, Mihai-Cristian Fera, Jose M. Abad, Antonio L. De Lacey, Marcos Pita

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Abstract

Oxidoreductase enzymes, used for a variety of applications including organic synthesis and pharmaceutical industry, require reduced nicotinamide adenine dinucleotide (NADH) as reducing equivalents. Methods for regenerating NAD⁺ to NADH are of significant interest due to the high cost and stoichiometric amounts of cofactor required. Diaphorase/redox mediator systems have shown promise for this purpose, but suitable mediators are few due to the low redox potential required, necessary downstream processing and stability issues. A novel amino-functionalized viologen is presented in this work which, upon immobilization with diaphorase, yields bioactive NADH with high selectivity (99 %) and faradaic efficiency (99 %). This system was tested with NADH-dependent formate dehydrogenase, showing a 21-fold improvement in formate yield compared to an enzymatic negative control without NADH regeneration. The findings underscore the potential of this novel amino-functionalized viologen polymer to advance sustainable and efficient NADH regeneration at very low overpotential.

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一种新型氨基功能化紫素氧化还原聚合物的高效生物电催化NADH再生

氧化还原酶用于包括有机合成和制药工业在内的各种应用，需要还原的烟酰胺腺嘌呤二核苷酸（NADH）作为还原当量。将NAD+再生为NADH的方法由于高成本和所需的辅助因子的化学计量量而引起了人们的极大兴趣。Diaphorase/氧化还原介质系统已显示出用于这一目的的希望，但由于所需的低氧化还原电位，必要的下游处理和稳定性问题，合适的介质很少。在这项工作中提出了一种新的氨基功能化的酶，在用二磷酸腺苷酶固定后，产生具有高选择性（99%）和法拉第效率（99%）的生物活性NADH。用NADH依赖性甲酸脱氢酶对该系统进行了测试，结果显示，与没有NADH再生的酶阴性对照相比，该系统的甲酸产量提高了21倍。这些发现强调了这种新型氨基功能化紫素聚合物在极低过电位下促进可持续和有效的NADH再生的潜力。

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来源期刊

Bioelectrochemistry 生物-电化学

CiteScore

9.10

自引率

6.00%

发文量

238

审稿时长

38 days

期刊介绍： An International Journal Devoted to Electrochemical Aspects of Biology and Biological Aspects of Electrochemistry Bioelectrochemistry is an international journal devoted to electrochemical principles in biology and biological aspects of electrochemistry. It publishes experimental and theoretical papers dealing with the electrochemical aspects of: • Electrified interfaces (electric double layers, adsorption, electron transfer, protein electrochemistry, basic principles of biosensors, biosensor interfaces and bio-nanosensor design and construction. • Electric and magnetic field effects (field-dependent processes, field interactions with molecules, intramolecular field effects, sensory systems for electric and magnetic fields, molecular and cellular mechanisms) • Bioenergetics and signal transduction (energy conversion, photosynthetic and visual membranes) • Biomembranes and model membranes (thermodynamics and mechanics, membrane transport, electroporation, fusion and insertion) • Electrochemical applications in medicine and biotechnology (drug delivery and gene transfer to cells and tissues, iontophoresis, skin electroporation, injury and repair). • Organization and use of arrays in-vitro and in-vivo, including as part of feedback control. • Electrochemical interrogation of biofilms as generated by microorganisms and tissue reaction associated with medical implants.