A 300-fold conductivity increase in microbial cytochrome nanowires due to temperature-induced restructuring of hydrogen bonding networks.

Autor: Dahl PJ; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Yi SM; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Gu Y; Microbial Sciences Institute, Yale University, New Haven, CT, USA.; Department of Molecular, Cellular and Developmental Biology, Yale University, New Haven, CT, USA., Acharya A; Department of Chemistry, Yale University, New Haven, CT, USA., Shipps C; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Neu J; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., O'Brien JP; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Morzan UN; Department of Chemistry, Yale University, New Haven, CT, USA., Chaudhuri S; Department of Chemistry, Yale University, New Haven, CT, USA., Guberman-Pfeffer MJ; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Vu D; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Yalcin SE; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA., Batista VS; Department of Chemistry, Yale University, New Haven, CT, USA., Malvankar NS; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, CT, USA.; Microbial Sciences Institute, Yale University, New Haven, CT, USA.
Jazyk: angličtina
Zdroj: Science advances [Sci Adv] 2022 May 13; Vol. 8 (19), pp. eabm7193. Date of Electronic Publication: 2022 May 11.
DOI: 10.1126/sciadv.abm7193
Abstrakt: Although proteins are considered as nonconductors that transfer electrons only up to 1 to 2 nanometers via tunneling, Geobacter sulfurreducens transports respiratory electrons over micrometers, to insoluble acceptors or syntrophic partner cells, via nanowires composed of polymerized cytochrome OmcS. However, the mechanism enabling this long-range conduction is unclear. Here, we demonstrate that individual nanowires exhibit theoretically predicted hopping conductance, at rate (>10 10 s -1 ) comparable to synthetic molecular wires, with negligible carrier loss over micrometers. Unexpectedly, nanowires show a 300-fold increase in their intrinsic conductance upon cooling, which vanishes upon deuteration. Computations show that cooling causes a massive rearrangement of hydrogen bonding networks in nanowires. Cooling makes hemes more planar, as revealed by Raman spectroscopy and simulations, and lowers their reduction potential. We find that the protein surrounding the hemes acts as a temperature-sensitive switch that controls charge transport by sensing environmental perturbations. Rational engineering of heme environments could enable systematic tuning of extracellular respiration.
Databáze: MEDLINE
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