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Light as Trigger for Biocatalysis: Photonic Wiring of Flavin Adenine Dinucleotide-Dependent Glucose Dehydrogenase to Quantum Dot-Sensitized Inverse Opal TiO2 Architectures via Redox Polymers

Title:
Light as Trigger for Biocatalysis: Photonic Wiring of Flavin Adenine Dinucleotide-Dependent Glucose Dehydrogenase to Quantum Dot-Sensitized Inverse Opal TiO2 Architectures via Redox Polymers
Abstract:
The functional coupling of photoactive nanostructures with enzymes creates a strategy for the design of light-triggered biocatalysts. This study highlights the efficient wiring of flavin adenine dinucleotide (FAD)-dependent glucose dehydrogenase (FAD-GDH) to PbS quantum dot (QD)-sensitized inverse opal TiO2 electrodes (IO-TiO2) by means of an Os-complex-containing redox polymer for the light-driven glucose oxidation. For the construction of IO-TiO2 scaffolds, a template approach has been developed, enabling the tunability of the surface area and a high loading capacity for the integration of QDs, redox polymer, and enzyme. The biohybrid signal chain can be switched on with light, generating charge carriers within the QDs, triggering a multistep electron-transfer cascade from the enzyme toward the redox polymer via the QDs and finally to the IO-TiO2 electrode. The resulting anodic photocurrent can be modulated by the potential, the excitation intensity, and the glucose concentration, providing a new degree of freedom for the control of biocatalyic reactions at electrode interfaces. Maximum photocurrents of 207 μA cm–2 have been achieved in the presence of glucose, and a first gain of electrons from the biocatalytic reaction is found at −540 mV vs Ag/AgCl, 1 M KCl, which lowers the working potential by >500 mV as compared to light-insensitive electrodes. The biohybrid system combines the advantages of a high surface area of IO films, an efficient charge-carrier generation and separation at the QDs/TiO2 interface, and an efficient wiring of FAD-GDH to the QDs via a redox polymer, resulting in photo(bio)anodes of high performance for sensing and power supply.
Year:
2018
Publication type:
Journal article
Journal:
ACS Catalysis
ISSN:
2155-5435
Number:
6
Volume:
8
Pages:
5212–5220
Language:
English
Document status:
Published
PubListerURL:
https://publister.bib.th-wildau.de/publister/public/publication/2578
Keywords:
Keywords: biocatalysis; enzymes; osmium polymer; photobioelectrochemical fuel cells; photoelectrochemical sensor; quantum dots
Riedel, M., Parak, W., Ruff, A., Schuhmann, W., & Lisdat, F. (2018). Light as Trigger for Biocatalysis: Photonic Wiring of Flavin Adenine Dinucleotide-Dependent Glucose Dehydrogenase to Quantum Dot-Sensitized Inverse Opal TiO2 Architectures via Redox Polymers ACS Catalysis. 8 (6), 5212–5220.
@article{2578,
    author           = {Riedel, Marc and Parak, Wolfgang J. and Ruff, Adrian and Schuhmann, Wolfgang and Lisdat, Fred},
    title            = {Light as Trigger for Biocatalysis: Photonic Wiring of Flavin Adenine Dinucleotide-Dependent Glucose Dehydrogenase to Quantum Dot-Sensitized Inverse Opal TiO2 Architectures via Redox Polymers},
    journal          = {ACS Catalysis},
    year             = {2018},
    volume           = {8},
    number           = {6},
    pages            = {5212–5220},
    publisher        = {American Chemical Society (ACS)},
    doi              = {10.1021/acscatal.8b00951},
}


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