Semiartificial photosynthetic nanoreactors for H2 generation

Zhang, Huijie, Jaenecke, Jan, Bishara-Robertson, Imogen L., Casadevall, Carla, Redman, Holly J., Winkler, Martin, Berggren, Gustav, Plumeré, Nicolas, Butt, Julea N. ORCID: https://orcid.org/0000-0002-9624-5226, Reisner, Erwin and Jeuken, Lars J. C. (2024) Semiartificial photosynthetic nanoreactors for H2 generation. Journal of the American Chemical Society, 146 (50). 34260–34264. ISSN 0002-7863

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Abstract

A relatively unexplored energy source in synthetic cells is transmembrane electron transport, which like proton and ion transport can be light driven. Here, synthetic cells, called nanoreactors, are engineered for compartmentalized, semiartificial photosynthetic H2 production by a Clostridium beijerinckii [FeFe]-hydrogenase (H2ase). Transmembrane electron transfer into the nanoreactor was enabled by MtrCAB, a multiheme transmembrane protein from Shewanella oneidensis MR-1. On illumination, graphitic nitrogen-doped carbon dots (g-N-CDs) outside the nanoreactor generated and delivered photoenergized electrons to MtrCAB, which transferred these electrons to encapsulated H2ase without requiring redox mediators. Compartmentalized, light-driven H2 production was observed with a turnover frequency (TOFH2ase) of 467 ± 64 h–1 determined in the first 2 h. Addition of the redox mediator methyl viologen (MV) increased TOFH2ase to 880 ± 154 h–1. We hypothesize that the energetically “uphill” electron transfer step from MtrCAB to H2ase ultimately limits the catalytic rate. These nanoreactors provide a scaffold to compartmentalize redox half reactions in semiartificial photosynthesis and inform on the engineering of nanoparticle–microbe hybrid systems for solar-to-chemical conversion.

Item Type:	Article
Additional Information:	Funding information: The authors acknowledge the UK Biotechnology and Biological Sciences Research Council for funding (BB/S002499/1, BB/S00159X/1, and BB/S000704/1). Financial support was provided by a BMBF project SynHydro3 (031B1123A) to N.P. and to M.W. (031B1123C). N.P. was further funded by the FNR project SynergyFuels (16RK34003K). Jan Jaenecke acknowledges financial support by “The German Academic Scholarship Foundation”.
Uncontrolled Keywords:	3* ,/dk/atira/pure/researchoutput/REFrank/3_
Faculty \ School:	Faculty of Science > School of Biological Sciences
UEA Research Groups:	Faculty of Science > Research Groups > Centre for Photonics and Quantum Science Faculty of Science > Research Groups > Molecular Microbiology Faculty of Science > Research Groups > Energy Materials Laboratory Faculty of Science > Research Groups > Chemistry of Light and Energy Faculty of Science > Research Groups > Chemistry of Life Processes Faculty of Science > Research Centres > Centre for Molecular and Structural Biochemistry
Related URLs:	https://pubs.acs.org/doi/full/10.1021/ja...
Depositing User:	LivePure Connector
Date Deposited:	06 Dec 2024 01:42
Last Modified:	21 Dec 2024 01:11
URI:	https://ueaeprints.uea.ac.uk/id/eprint/97922
DOI:	10.1021/jacs.4c12311

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