Rational design of covalent multiheme cytochrome-graphitic carbon dot biohybrids for photo-induced electron transfer

Zhang, Huijie, Casadevall, Carla, van Wonderen, Jessica H., Su, Lin, Butt, Julea N. ORCID: https://orcid.org/0000-0002-9624-5226, Reisner, Erwin and Jeuken, Lars J. C. (2023) Rational design of covalent multiheme cytochrome-graphitic carbon dot biohybrids for photo-induced electron transfer. Advanced Functional Materials, 33 (40). ISSN 1616-301X

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Biohybrid systems can combine inorganic light-harvesting materials and whole-cell biocatalysts to utilize solar energy for the production of chemicals and fuels. Whole-cell biocatalysts have an intrinsic self-repair ability and are able to produce a wide variety of multicarbon chemicals in a sustainable way with metabolic engineering. Current whole-cell biohybrid systems have a yet undefined electron transfer pathway between the light-absorber and metabolic enzymes, limiting rational design. To enable engineering of efficient electron transfer pathways, covalent biohybrids consisting of graphitic nitrogen doped carbon dots (g-N-CDs) and the outer-membrane decaheme protein, MtrC from Shewanella oneidensis MR-1 are developed. MtrC is a subunit of the MtrCAB protein complex, which provides a direct conduit for bidirectional electron exchange across the bacterial outer membrane. The g-N-CDs are functionalized with a maleimide moiety by either carbodiimide chemistry or acyl chloride activation and coupled to a surface-exposed cysteine of a Y657C MtrC mutant. MtrC∼g-N-CD biohybrids are characterized by native and denaturing gel electrophoresis, chromatography, microscopy, and fluorescence lifetime spectroscopy. In the presence of a sacrificial electron donor, visible light irradiation of the MtrC∼g-N-CD biohybrids results in reduced MtrC. The biohybrids may find application in photoinduced transmembrane electron transfer in S. oneidensis MR-1 for chemical synthesis in the future.

Item Type: Article
Additional Information: Research Funding: UK Biotechnology and Biological Sciences Research Council. Grant Number: BB/S002499/1, BB/S00159X/1,and BB/S000704/1; EPSRC Multi-User Equipment Call. Grant Number: EP/P030467/1; European Commission. Grant Number: Marie Sklodowska-Curie Individual Fellowship 890745-SmArtC
Uncontrolled Keywords: biohybrids,covalent protein labeling,nanoparticles,semiartificial photosynthesis,solar fuels,electronic, optical and magnetic materials,chemistry(all),biomaterials,materials science(all),condensed matter physics,electrochemistry ,/dk/atira/pure/subjectarea/asjc/2500/2504
Faculty \ School: Faculty of Science > School of Chemistry
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
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Depositing User: LivePure Connector
Date Deposited: 25 May 2023 10:32
Last Modified: 12 Oct 2023 00:41
URI: https://ueaeprints.uea.ac.uk/id/eprint/92186
DOI: 10.1002/adfm.202302204


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