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

Journal article (2019)

Authors

Da Som Choi Korea Advanced Institute of Science and Technology
Hojin Lee Korea Advanced Institute of Science and Technology
F. Tieves BT/Biocatalysis - AS
Yang Woo Lee Korea Advanced Institute of Science and Technology
Eun Jin Son Korea Advanced Institute of Science and Technology
W. Zhang BT/Biocatalysis - AS
Byungha Shin Korea Advanced Institute of Science and Technology
Frank Hollmann BT/Biocatalysis - AS
F. Hollmann BT/Biocatalysis - AS
Chan Beum Park Korea Advanced Institute of Science and Technology
Research Group
BT/Biocatalysis (AS) (TU Delft)
Copyright: © 2019 Da Som Choi, Hojin Lee, F. Tieves, Yang Woo Lee, Eun Jin Son, W. Zhang, Byungha Shin, F. Hollmann, Chan Beum Park
DOI: https://doi.org/10.1021/acscatal.9b04454
More Info
expand_more

Published Date

2019

Language

English

Reuse Rights

Other than for strictly personal use, it is not permitted to download, forward or distribute the text or part of it, without the consent of the author(s) and/or copyright holder(s), unless the work is under an open content license such as Creative Commons.

Faculty

Applied Sciences

Department

BT/Biotechnologie

Research Group

BT/Biocatalysis

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.

Files

Acscatal.9b04454.pdf
(pdf | 1.52 Mb)
- Embargo expired in 15-04-2020
Unknown license