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Light-Driven Catalytic Upgrading of Butanol in a Biohybrid Photoelectrochemical System
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    Light-Driven Catalytic Upgrading of Butanol in a Biohybrid Photoelectrochemical System
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    † ‡ Department of Chemical and Biological Engineering and Materials Science and Engineering Program, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303, United States
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    ACS Sustainable Chemistry & Engineering

    Cite this: ACS Sustainable Chem. Eng. 2017, 5, 9, 8199–8204
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    https://doi.org/10.1021/acssuschemeng.7b01849
    Published July 18, 2017
    Copyright © 2017 American Chemical Society

    Abstract

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    This paper reports the design and preparation of a biohybrid photoelectrochemical cell (PEC) that can drive the tandem enzymatic oxidation and aldol condensation of n-butanol (BuOH) to C8 2-ethylhexenal (2-EH). In this work, BuOH was first oxidized to n-butyraldehyde (BA) by the alcohol oxidase enzyme (AOx), concurrently generating hydrogen peroxide (H2O2). To preserve enzyme activity and increase kinetics nearly 2-fold, the H2O2 was removed by oxidation at a bismuth vanadate (BiVO4) photoanode. Organocatalyzed aldol condensation of C4 BA to C8 2-EH improved the overall BuOH conversion to 6.2 ± 0.1% in a biased PEC after 16 h. A purely light-driven, unbiased PEC showed 3.1 ± 0.1% BuOH conversion, or ∼50% of that obtained from the biased system. Replacing AOx with the enzyme alcohol dehydrogenase (ADH), which requires the diffusional nicotinamide adenine dinucleotide cofactor (NAD+/NADH), resulted in only 0.2% BuOH conversion due to NAD+ dimerization at the photoanode. Lastly, the application of more positive biases with the biohybrid AOx PEC led to measurable production of H2 at the cathode, but at the cost of lower BA and 2-EH yields due to both product overoxidation and decreased enzyme activity.

    Copyright © 2017 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acssuschemeng.7b01849.

    • UV–vis spectra of BiVO4, LSV measurements, product extraction partitioning coefficients curves, 1H NMR spectra of extracted products, ADH reaction results, hydroxyl radical formation verification tests, AOx reaction yields at varying biases, BiVO4 electrodeposition data, the gas chromatograph calibration curve, enzyme control experiments, and a summary of results table (PDF)

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    ACS Sustainable Chemistry & Engineering

    Cite this: ACS Sustainable Chem. Eng. 2017, 5, 9, 8199–8204
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acssuschemeng.7b01849
    Published July 18, 2017
    Copyright © 2017 American Chemical Society

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