Rational wiring of photosystem II to hierarchical indium tin oxide electrodes using redox polymers

Sokol, Katarzyna P.; Mersch, Dirk; Hartmann, Volker; Zhang, Jenny; Nowaczyk, Marc M.; Rögner, Matthias; Ruff, Adrian; Schuhmann, Wolfgang; Plumeré, Nicolas; Reisner, Erwin

doi:10.1039/c6ee01363e

Cited by 151 publications

(184 citation statements)

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“…The rather low redox potential of the polymer‐bound phenothiazine moieties ensures a high OCV of the corresponding biofuel cell. However, at these negative potentials undesired O 2 reduction at the anode side might become an issue . Thus, the potential of the mediator has to be adjusted by means of a careful design of the redox polymer (vide infra).…”

Section: Resultsmentioning

confidence: 99%

“…The combination of such a biocathode with an NAD + ‐dependent ADH‐based bioanode should provide a high OCV if a low potential redox mediator (e. g. redox dyes or quniones) is used for the oxidation of NADH at the anode. Polymer‐bound phenothiazine dyes which are reduced at rather negative potentials in a 2e − / n H + step to their corresponding leuco forms (where n is the number of transferred protons and depends on the pH value) are well known redox mediators for the regeneration of NAD +[37–43] and were used earlier for the fabrication of polymer‐based low potential bioanodes . Thus, we considered such bioanodes as promising candidates for the design of enzyme electrodes comprising NAD + ‐dependent ADH as biological selectivity element.…”

Section: Introductionmentioning

confidence: 99%

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A Self‐Powered Ethanol Biosensor

et al. 2017

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We describe the fabrication of a self‐powered ethanol biosensor comprising a β‐NAD+‐dependent alcohol dehydrogenase (ADH) bioanode and a bienzymatic alcohol oxidase (AOx) and horseradish peroxidase (HRP) biocathode. β‐NAD+ is regenerated by means of a specifically designed phenothiazine dye (i. e. toluidine blue, TB) modified redox polymer in which TB was covalently anchored to a hexanoic acid tethered poly(4‐vinylpyridine) backbone. The redox polymer acts as an immobilization matrix for ADH. Using a carefully chosen anchoring strategy through the formation of amide bonds, the potential of the TB‐based mediator is shifted to more positive potentials, thus preventing undesired O2 reduction. To counterbalance the rather high potential of the TB‐modified polymer, and thus the bioanode, a high‐potential AOx/HRP‐based biocathode is suggested. HRP is immobilized in a direct‐electron‐transfer regime on screen‐printed graphite electrodes functionalized with multi‐walled carbon nanotubes. The nanostructured cathode ensures the wiring of the iron‐oxo complex within oxidized HRP, and thus a high potential for the reduction of H2O2 of about +550 mV versus Ag/AgCl/3 M KCl. The proposed biofuel cell exhibits an open‐circuit voltage (OCV) of approximately 660 mV and was used as self‐powered device for the determination of the ethanol content in liquor.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

A Self‐Powered Ethanol Biosensor

et al. 2017

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“…Diese Plattformen bençtigen aber (zusätzlich zu Lichtenergie) oft eine hohe externe Vorspannung,u ms owohl die Wasseroxidation als auch die enzymatische Reduktion zu katalysieren. Der Einbau von Redoxenzymen in die als Photoelektroden verwendeten Materialien (wie beispielsweise in nanostrukturierte Gerüste [62,193] oder leitende Polymere [53,194,195] )kann die Elektronentransferpfade verkürzen, indem ein direkter Tr ansfer von der Photokathode zum aktiven Zentrum ermçglicht wird. Fürd ie weitere Entwicklung von Solarplattformen, die ohne externe Vorspannung arbeiten, sind ein rationales Design der Elektrodenmaterialien sowie ein geeigneter Aufbau der PECs unumgänglich.…”

Section: Verringerung Der Angelegten Vorspannung In Biokatalytischen unclassified

Photobiokatalyse: Aktivierung von Redoxenzymen durch direkten oder indirekten Transfer photoinduzierter Elektronen

et al. 2018

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Biokatalytische Umsetzungen rücken aufgrund der Vielfältigkeit der Enzyme, ihrer hohen katalytischen Aktivität und Spezifität und der milden Reaktionsbedingungen zunehmend in den Fokus einer “grünen” Synthesechemie. Der Ansatz, Sonnenenergie durch Kombination von Photokatalyse und Biokatalyse für die chemische Synthese nutzbar zu machen, bietet eine Möglichkeit, diesen “grünen” Prozess noch nachhaltiger zu gestalten. Oxidoreduktasen katalysieren die Umsetzung verschiedener Substrate durch den Austausch von Elektronen am aktiven Zentrum des Enzyms, meist mithilfe von Elektronenmediatoren. Aktuelle Fortschritte auf diesem Gebiet zeigen, dass photoinduzierter Elektronentransfer unter Einsatz organischer (oder anorganischer) Photosensibilisatoren ein breites Spektrum von Redoxenzymen aktivieren kann, welche in Folge wichtige Brennstoffe liefern (z. B. H2‐Bildung, CO2‐Reduktion) oder synthetisch relevante Reduktionen vermitteln (z. B. asymmetrische Reduktionen, Oxygenierungen, Hydroxylierungen, Epoxidierungen, Bayer‐Villiger‐Oxidation). Dieser Aufsatz gibt einen Überblick über aktuelle Entwicklungen auf dem Gebiet der Photoaktivierung von Redoxenzymen mittels direkter oder indirekter Übertragung photoinduzierter Elektronen.

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“…In this system, the laccase is able to oxidize the water to produce electricity at very low applied potential under sun illumination. The proximity between the laccase and the inorganic artificial cofactor (In 2 S 3 particles) enables the light‐driven water splitting reaction with catalytic constants similar to the best systems reported for photobioelectrical systems (Figure ).…”

Section: Irreversible Co‐immobilization Of Cofactor and Enzymes On Somentioning

confidence: 99%

Heterogeneous Systems Biocatalysis: The Path to the Fabrication of Self‐Sufficient Artificial Metabolic Cells

López‐Gallego

Jackson

Betancor

2017

Chemistry A European J

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Industrial biocatalysis is playing a key role in the development of the global bio-economy that must change our current productive model to pair the socio-economical development with the preservation of our already harmed planet. The exploitation of isolated multi-enzyme systems and the discovery of novel biocatalytic activities are leading us to manufacture chemicals that were inaccessible through biological routes in the early past. These endeavors have been grouped under the concept of systems biocatalysis. However, by using isolated biological machineries, fundamental features underlying the protein confinement found inside the living cells are missed. To re-gain these properties, such concepts can be expanded to a new concept; heterogeneous systems biocatalysis. This new concept is based on the fabrication of heterogeneous biocatalysts inspired by the spatial organization and compartmentalization that orchestrate metabolic pathways within cells. By assembling biological machineries (including enzymes and cofactors) into artificial solid chassis, one can fabricate self-sufficient and robust cell-free systems able to catalyze orchestrated chemical processes. Furthermore, the confinement of enzymes and and "artificial cofactor" inside solid materials has also attracted our attention because these self-sufficient systems exert de novo and non-natural functionalities. Here, we intend to go beyond immobilization of multi-enzyme systems, discussing only those enzymatic systems that have been co-immobilized with their cofactor or exogenous partners to enhance their cooperative action. In this article, we review the latest architectures developed to fabricate self-sufficient heterogeneous biocatalysts with application in chemical manufacturing, biosensing or energy production.

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Rational wiring of photosystem II to hierarchical indium tin oxide electrodes using redox polymers

Abstract: A rational approach for a photosystem II-based electrode assembly is described, integrating redox polymers with high surface area hierarchically structured electrodes.

Cited by 151 publications

References 54 publications

A Self‐Powered Ethanol Biosensor

A Self‐Powered Ethanol Biosensor

Photobiokatalyse: Aktivierung von Redoxenzymen durch direkten oder indirekten Transfer photoinduzierter Elektronen

Heterogeneous Systems Biocatalysis: The Path to the Fabrication of Self‐Sufficient Artificial Metabolic Cells

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