Bias-Free in Situ H2O2 Generation in a Photovoltaic-Photoelectrochemical Tandem Cell for Biocatalytic Oxyfunctionalization

Title

Bias-Free in Situ H2O2 Generation in a Photovoltaic-Photoelectrochemical Tandem Cell for Biocatalytic Oxyfunctionalization

 Author

Choi, Da Som (Korea Advanced Institute of Science and Technology)
Lee, Hojin (Korea Advanced Institute of Science and Technology)
Tieves, F. (TU Delft BT/Biocatalysis)
Lee, Yang Woo (Korea Advanced Institute of Science and Technology)
Son, Eun Jin (Korea Advanced Institute of Science and Technology)
Zhang, W. (TU Delft BT/Biocatalysis) ORCID 0000-0002-3182-5107
Shin, Byungha (Korea Advanced Institute of Science and Technology)
Hollmann, F. (TU Delft BT/Biocatalysis) ORCID 0000-0003-4821-756X
Park, Chan Beum (Korea Advanced Institute of Science and Technology)

Date

2019

 Abstract

Peroxygenases catalyze selective oxyfunctionalization of hydrocarbons with high conversion efficiencies using H2O2 as a key cosubstrate. Here, we report an unbiased photoelectrochemical (PEC) tandem structure consisting of a FeOOH/BiVO4 photoanode, a Cu(In,Ga)Se2 solar absorber, and a graphitic carbon nitride/reduced graphene oxide hybrid cathode for light-driven peroxygenase catalysis. Powered by sufficient photovoltage generated by the solar absorber, the PEC platform generates H2O2 in situ through reductive activation of molecular oxygen using water as an electron donor in the absence of external bias. The peroxygenase from Agrocybe aegerita catalyzed the stereoselective hydroxylation of ethylbenzene to (R)-1-phenylethanol with total turnover numbers over 43 300 and high enantioselectivity (ee > 99%) in the unbiased PEC tandem system.


 Subject

biocatalysis
oxyfunctionalization
peroxygenases
photoelectrochemical cells
photovoltaics

 To reference this document use:

http://resolver.tudelft.nl/uuid:2894d012-d561-4e2b-88cc-ff54dacf3914

 DOI

https://doi.org/10.1021/acscatal.9b04454

 Embargo date

2020-04-15

 ISSN

2155-5435

 Source

ACS Catalysis, 9 (11), 10562-10566

 Bibliographical note

Green Open Access added to TU Delft Institutional Repository ‘You share, we take care!’ – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

 Part of collection

Institutional Repository

 Document type

journal article

 Rights

© 2019 Da Som Choi, Hojin Lee, F. Tieves, Yang Woo Lee, Eun Jin Son, W. Zhang, Byungha Shin, F. Hollmann, Chan Beum Park
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