Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H<sub>2</sub>oxidation at low overpotential

Oughli, Alaa A.; Vélez, Marisela; Birrell, James A.; Schuhmann, Wolfgang; Lubitz, Wolfgang; Plumeré, Nicolas; Rüdiger, Olaf

doi:10.1039/c8dt00955d

Cited by 10 publications

(9 citation statements)

References 46 publications

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“…Various ligands were synthesized to tune the redox potentials of the hydrogels. 593 A similar viologen polymer-modified bioelectrode has been reported by Kano's group for formate oxidation by FDH, and a formate/O 2 EFC with an OCV of 1.2 V was recorded. 15 Compared to the DET-type bioelectrocatalysis and MET-type bioelectrocatalysis using free mediators, redox polymer-based bioelectrocatalysis possess advantages such as rapid rates of ET, low levels of mediators and/or enzyme leakage.…”

Section: Chemical Reviewssupporting

confidence: 64%

“… H 2 /O 2 EFCs with high OCVs of ∼1 V were fabricated by combination of such viologen-based polymer MET-type H 2 bioanodes and DET-type O 2 biocathodes. Various ligands were synthesized to tune the redox potentials of the hydrogels . A similar viologen polymer-modified bioelectrode has been reported by Kano’s group for formate oxidation by FDH, and a formate/O 2 EFC with an OCV of 1.2 V was recorded .…”

Section: Approaches For the Improvement Of Efcs’ Cell Voltagementioning

confidence: 95%

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Tackling the Challenges of Enzymatic (Bio)Fuel Cells

et al. 2019

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The ever-increasing demands for clean and sustainable energy sources combined with rapid advances in bio-integrated portable or implantable electronic devices have stimulated intensive research activities in enzymatic (bio)fuel cells (EFCs). The use of renewable biocatalysts, the utilization of abundant green, safe, and high energy density fuels, together with the capability of working at modest and biocompatible conditions, make EFCs promising as next generation alternative power sources. However, the main challenges (low energy density, relatively low power density, poor operational stability and limited voltage output) hinder future applications of EFCs. This review aims at exploring the underlying mechanism of EFCs and providing possible practical strategies, methodologies and insights to tackle of these issues. Firstly, this review summarizes approaches in achieving high energy densities in EFCs, particularly, employing enzyme cascades for the deep/complete oxidation of fuels. Secondly, strategies for increasing power densities in EFCs, including increasing enzyme activities, facilitating electron transfers, employing nanomaterials, and designing more efficient enzyme-electrode interfaces, are described. The potential of EFCs/(super)capacitor combination is discussed. Thirdly, the review evaluates a range of strategies for improving the stability of EFCs, including the use of different enzyme immobilization approaches, tuning enzyme properties, designing protective matrixes, and using microbial surface displaying enzymes. Fourthly, approaches for the improvement of the cell voltage of EFCs are highlighted. Finally, future developments and a prospective on EFCs are envisioned.

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Section: Chemical Reviewssupporting

confidence: 64%

Section: Approaches For the Improvement Of Efcs’ Cell Voltagementioning

confidence: 95%

Tackling the Challenges of Enzymatic (Bio)Fuel Cells

et al. 2019

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“…In addition, redox polymers can serve as a protection against oxygen for oxygen-sensitive enzymes, , unwanted contributions from DET of contaminants, and high potential deactivations, that are limiting factors in further improving enzyme-based applications . Specifically, Szczesny et al built a bioanode using the viologen-modified redox polymers to mediate hydrogenase .…”

Section: The Bioelectrocatalysis Systemmentioning

confidence: 99%

Fundamentals, Applications, and Future Directions of Bioelectrocatalysis

et al. 2020

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Bioelectrocatalysis is an interdisciplinary research field combining biocatalysis and electrocatalysis via the utilization of materials derived from biological systems as catalysts to catalyze the redox reactions occurring at an electrode. Bioelectrocatalysis synergistically couples the merits of both biocatalysis and electrocatalysis. The advantages of biocatalysis include high activity, high selectivity, wide substrate scope, and mild reaction conditions. The advantages of electrocatalysis include the possible utilization of renewable electricity as an electron source and high energy conversion efficiency. These properties are integrated to achieve selective biosensing, efficient energy conversion, and the production of diverse products. This review seeks to systematically and comprehensively detail the fundamentals, analyze the existing problems, summarize the development status and applications, and look toward the future development directions of bioelectrocatalysis. First, the structure, function, and modification of bioelectrocatalysts are discussed. Second, the essentials of bioelectrocatalytic systems, including electron transfer mechanisms, electrode materials, and reaction medium, are described. Third, the application of bioelectrocatalysis in the fields of biosensors, fuel cells, solar cells, catalytic mechanism studies, and bioelectrosyntheses of high-value chemicals are systematically summarized. Finally, future developments and a perspective on bioelectrocatalysis are suggested.

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“…Alternatively, it was shown that embedding the hydrogenase in a viologen-based hydrogel protected the enzyme from high potential deactivation. In this MET process, the enzyme no longer senses the high potential of the electrode but the potential of the viologen redox couple which is sufficiently negative to prevent HASE inactivation [287][288][289]. Nevertheless, the use of redox mediators induces other detrimental effects towards enzyme stability, such as production of reactive oxygen species (ROS) that will be discussed in the next section.…”

Section: Effect Of the Electric Fieldmentioning

confidence: 99%

From Enzyme Stability to Enzymatic Bioelectrode Stabilization Processes

et al. 2021

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Bioelectrocatalysis using redox enzymes appears as a sustainable way for biosensing, electricity production, or biosynthesis of fine products. Despite advances in the knowledge of parameters that drive the efficiency of enzymatic electrocatalysis, the weak stability of bioelectrodes prevents large scale development of bioelectrocatalysis. In this review, starting from the understanding of the parameters that drive protein instability, we will discuss the main strategies available to improve all enzyme stability, including use of chemicals, protein engineering and immobilization. Considering in a second step the additional requirements for use of redox enzymes, we will evaluate how far these general strategies can be applied to bioelectrocatalysis.

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Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H₂oxidation at low overpotential

Abstract: In this work we present a viologen-modified electrode providing protection for hydrogenases against high potential inactivation.

Cited by 10 publications

References 46 publications

Tackling the Challenges of Enzymatic (Bio)Fuel Cells

Tackling the Challenges of Enzymatic (Bio)Fuel Cells

Fundamentals, Applications, and Future Directions of Bioelectrocatalysis

From Enzyme Stability to Enzymatic Bioelectrode Stabilization Processes

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Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H2oxidation at low overpotential

Abstract: In this work we present a viologen-modified electrode providing protection for hydrogenases against high potential inactivation.

Cited by 10 publications

References 46 publications

Tackling the Challenges of Enzymatic (Bio)Fuel Cells

Tackling the Challenges of Enzymatic (Bio)Fuel Cells

Fundamentals, Applications, and Future Directions of Bioelectrocatalysis

From Enzyme Stability to Enzymatic Bioelectrode Stabilization Processes

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Product

Resources

About

Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H₂oxidation at low overpotential