Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase
Hydrogen peroxide (H₂O₂) is a strong oxidizing agent that is commonly employed in chemical synthesis. Nevertheless, its utilization as a cosubstrate in biocatalytic reactions remains limited due to the deactivating effect on biocatalysts at an elevated concentration. An electrochemical synthesis of...
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Elsevier
2025-08-01
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| Series: | Electrochemistry Communications |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S1388248125000888 |
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| author | Giovanni V. Sayoga Victoria S. Bueschler Hubert Beisch Bodo Fiedler Daniel Ohde Andreas Liese |
| author_facet | Giovanni V. Sayoga Victoria S. Bueschler Hubert Beisch Bodo Fiedler Daniel Ohde Andreas Liese |
| author_sort | Giovanni V. Sayoga |
| collection | DOAJ |
| description | Hydrogen peroxide (H₂O₂) is a strong oxidizing agent that is commonly employed in chemical synthesis. Nevertheless, its utilization as a cosubstrate in biocatalytic reactions remains limited due to the deactivating effect on biocatalysts at an elevated concentration. An electrochemical synthesis of H₂O₂ represents an attractive approach, offering a controllable in situ generation of H₂O₂ without producing complex by-products. The objective of this study is to demonstrate the feasibility of the in situ electrogeneration of H₂O₂ using the All-in-One (AiO) electrode within a flow reactor technology. Integrating a bioelectrochemical system (BES) into a flow reactor technology, such as a flow cell, presents an alternative strategy for scale-up. In this study, the in situ generation of H₂O₂ is coupled with the hydroxylation of 4-ethylbenzoic acid catalyzed by the immobilized recombinant unspecific peroxygenase from Agrocybe aegerita (rAaeUPO) within a complete BES under batch and fed-batch operation modes. The electrochemical flow cell facilitates a controllable H₂O₂ generation by adjusting experimental parameters such as current density, aeration rate and residence time. The flow cell BES equipped with the AiO electrode yielded a catalytic productivity as high as 1.24 ± 0.02 mM h−1 (4.95 ± 0.1 g L−1 d−1), a total turnover number of rAaeUPO up to 3.38 · 105 ± 702 mol mol−1 and a turnover frequency up to 8.34 ± 0.14 s−1. |
| format | Article |
| id | doaj-art-463b27a577674a18a3b21f154e02ff37 |
| institution | DOAJ |
| issn | 1388-2481 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Electrochemistry Communications |
| spelling | doaj-art-463b27a577674a18a3b21f154e02ff372025-08-20T02:48:39ZengElsevierElectrochemistry Communications1388-24812025-08-0117710794910.1016/j.elecom.2025.107949Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenaseGiovanni V. Sayoga0Victoria S. Bueschler1Hubert Beisch2Bodo Fiedler3Daniel Ohde4Andreas Liese5Institute of Technical Biocatalysis, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, Germany; Corresponding authors at: Institute of Technical Biocatalysis, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, Germany.Institute of Technical Biocatalysis, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, GermanyInstitute of Polymers and Composites, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, GermanyInstitute of Polymers and Composites, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, GermanyInstitute of Technical Biocatalysis, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, GermanyInstitute of Technical Biocatalysis, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, Germany; Corresponding authors at: Institute of Technical Biocatalysis, Hamburg University of Technology, Denickestraße 15, 21073 Hamburg, Germany.Hydrogen peroxide (H₂O₂) is a strong oxidizing agent that is commonly employed in chemical synthesis. Nevertheless, its utilization as a cosubstrate in biocatalytic reactions remains limited due to the deactivating effect on biocatalysts at an elevated concentration. An electrochemical synthesis of H₂O₂ represents an attractive approach, offering a controllable in situ generation of H₂O₂ without producing complex by-products. The objective of this study is to demonstrate the feasibility of the in situ electrogeneration of H₂O₂ using the All-in-One (AiO) electrode within a flow reactor technology. Integrating a bioelectrochemical system (BES) into a flow reactor technology, such as a flow cell, presents an alternative strategy for scale-up. In this study, the in situ generation of H₂O₂ is coupled with the hydroxylation of 4-ethylbenzoic acid catalyzed by the immobilized recombinant unspecific peroxygenase from Agrocybe aegerita (rAaeUPO) within a complete BES under batch and fed-batch operation modes. The electrochemical flow cell facilitates a controllable H₂O₂ generation by adjusting experimental parameters such as current density, aeration rate and residence time. The flow cell BES equipped with the AiO electrode yielded a catalytic productivity as high as 1.24 ± 0.02 mM h−1 (4.95 ± 0.1 g L−1 d−1), a total turnover number of rAaeUPO up to 3.38 · 105 ± 702 mol mol−1 and a turnover frequency up to 8.34 ± 0.14 s−1.http://www.sciencedirect.com/science/article/pii/S1388248125000888BiocatalysisBioelectrochemical systemElectrosynthesisFlow reactorHydroxylationUnspecific peroxygenase |
| spellingShingle | Giovanni V. Sayoga Victoria S. Bueschler Hubert Beisch Bodo Fiedler Daniel Ohde Andreas Liese Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase Electrochemistry Communications Biocatalysis Bioelectrochemical system Electrosynthesis Flow reactor Hydroxylation Unspecific peroxygenase |
| title | Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase |
| title_full | Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase |
| title_fullStr | Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase |
| title_full_unstemmed | Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase |
| title_short | Integration of the All-in-One electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase |
| title_sort | integration of the all in one electrode in an electrochemical flow cell for in situ hydrogen peroxide supply in hydroxylation mediated by immobilized unspecific peroxygenase |
| topic | Biocatalysis Bioelectrochemical system Electrosynthesis Flow reactor Hydroxylation Unspecific peroxygenase |
| url | http://www.sciencedirect.com/science/article/pii/S1388248125000888 |
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