Issue 12, 2023

E. coli-based semi-artificial photosynthesis: biocompatibility of redox mediators and electron donors in [FeFe] hydrogenase driven hydrogen evolution

Abstract

Semi-artificial photosynthesis aims to harness the power of biocatalysis while breaking away from the limitations of Nature's photosynthetic machinery, by merging artificial light harvesters with enzyme catalysts. However, the artificial photocatalytic components are generally toxic towards the biological components. In this study, we investigate a system wherein Escherichia coli cells, heterologously expressing an [FeFe] hydrogenase, act as hydrogen evolution catalyst in combination with an artificial photosensitizer, sacrificial electron donor, and redox mediator. Previously, the use of artificial components or their reaction products was found to be toxic to E. coli cells. To overcome this challenge, we examined alternative electron donors and redox mediators, achieving turnover numbers (TON, 39.6 μmol H2 per 1 mL sample with OD600 = 5) and turnover frequencies (TOF, 812 nmol H2 h−1 per 1 mL sample with OD600 = 5) on par with previously reported high performing E. coli-based systems while greatly reducing cytotoxic effects. Transient absorption spectroscopy revealed how the choice of photosensitizer, electron donor, and redox mediator affects the observed photocatalytic TOFs. Following optimization of the redox mediator and electron donor the biocatalyst demonstrated remarkable stability throughout the experiments. We identified the availability of electrons from the electron donor as the primary limiting factor, with approximately 85% of electrons being effectively utilized for hydrogen production. Furthermore, the observed activity with different [FeFe] hydrogenases verified the broad applicability of the identified photocatalytic components to promote light-driven catalysis in bio-hybrid systems.

Graphical abstract: E. coli-based semi-artificial photosynthesis: biocompatibility of redox mediators and electron donors in [FeFe] hydrogenase driven hydrogen evolution

Supplementary files

Article information

Article type
Paper
Submitted
18 Sept. 2023
Accepted
03 Nov. 2023
First published
06 Nov. 2023
This article is Open Access
Creative Commons BY license

Energy Adv., 2023,2, 2085-2092

E. coli-based semi-artificial photosynthesis: biocompatibility of redox mediators and electron donors in [FeFe] hydrogenase driven hydrogen evolution

M. T. Gamache, L. Kurth, D. T. Filmon, N. Plumeré and G. Berggren, Energy Adv., 2023, 2, 2085 DOI: 10.1039/D3YA00462G

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