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

Da Som Choi, Hojin Lee, Florian Tieves, Yang Woo Lee, Eun Jin Son, Wuyuan Zhang, Byungha Shin, Frank Hollmann, Chan Beum Park*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

28 Citations (Scopus)
20 Downloads (Pure)

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.

Original languageEnglish
Pages (from-to)10562-10566
JournalACS Catalysis
Volume9
Issue number11
DOIs
Publication statusPublished - 2019

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.

Keywords

  • biocatalysis
  • oxyfunctionalization
  • peroxygenases
  • photoelectrochemical cells
  • photovoltaics

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