A1 Vertaisarvioitu alkuperäisartikkeli tieteellisessä lehdessä
Dissecting Bioelectrical Networks in Photosynthetic Membranes with Electrochemistry
Tekijät: Lawrence, Joshua M.; Egan, Rachel M.; Wey, Laura T.; Bali, Karan; Chen, Xiaolong; Kosmutzky, Darius; Eyres, Mairi; Nan, Lan; Wood, Mary H.; Nowaczyk, Marc M.; Howe, Christopher J.; Zhang, Jenny Z.
Kustantaja: American Chemical Society (ACS)
Kustannuspaikka: WASHINGTON
Julkaisuvuosi: 2025
Journal: Journal of the American Chemical Society
Tietokannassa oleva lehden nimi: Journal of the American Chemical Society
Lehden akronyymi: J AM CHEM SOC
Vuosikerta: 147
Numero: 30
Aloitussivu: 26907
Lopetussivu: 26916
Sivujen määrä: 10
ISSN: 0002-7863
eISSN: 1520-5126
DOI: https://doi.org/10.1021/jacs.5c08519
Verkko-osoite: https://doi.org/10.1021/jacs.5c08519
Rinnakkaistallenteen osoite: https://research.utu.fi/converis/portal/detail/Publication/499247721
Photosynthetic membranes contain complex networks of redox proteins and molecules, which direct electrons along various energy-to-chemical interconversion reactions important for sustaining life on Earth. Analyzing and disentangling the mechanisms, regulation, and interdependencies of these electron transfer pathways is extremely difficult, owing to the large number of interacting components in the native membrane environment. While electrochemistry is well established for studying electron transfer in purified proteins, it has proved difficult to wire into proteins within their native membrane environments and even harder to probe on a systems-level the electron transfer networks they are entangled within. Here, we show how photosynthetic membranes from cyanobacteria can be wired to electrodes to access their complex electron transfer networks. Measurements of native membranes with structured electrodes revealed distinctive electrochemical signatures, enabling analysis from the scale of individual proteins to entire biochemical pathways as well as their interplay. This includes measurements of overlapping photosynthetic and respiratory pathways, the redox activities of membrane-bound quinones, along with validation using in operando spectroscopic measurements. Importantly, we further demonstrated extraction of electrons from native membrane-bound Photosystem I at -600 mV versus SHE, which is similar to 1 V more negative than from purified photosystems. This finding opens up opportunities for biotechnologies for solar electricity, fuel, and chemical generation. We foresee this electrochemical method being adapted to analyze other photosynthetic and nonphotosynthetic membranes, as well as aiding the development of new biocatalytic, biohybrid, and biomimetic systems.
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The authors are grateful for support from the Biotechnology and Biological Sciences Research Council (BB/M011194/1 to J.M.L., BB/R011923/1 to J.Z.Z. & X.C.); the Worshipful Company of Leathersellers (J.M.L.); Trinity Hall, Cambridge (J.M.L.); the Novo Nordisk Foundation (NNF22OCOO79717 to L.T.W.); the Cambridge Trust (L.T.W., R.M.E., & L.N.); the Engineering and Physical Sciences Research Council (EP/R513180/1 to K.B.); Algae-UK (M.E.); the Chinese Scholarship Council (no. 202208060220 to L.N.); the Gates Cambridge Trust (D.G.K.); the Benn W Levy Trust (D.G.K.); the Human Frontiers Science Program (LT000307/2019 to M.H.W.); and the Deutsche Forschungsgemeinschaft (321933041 to M.M.N.) as part of the Research Training Group GRK 2341, "Microbial Substrate Conversion (MiCon)". The authors would like to thank Nicholas Plumere and Henry Lloyd-Laney for helpful discussions.
