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- W4200311938 abstract "In photosystem II (PSII), Cl- is a prerequisite for the second flash-induced oxidation of the Mn4CaO5 cluster (the S2 to S3 transition). We report proton transfer from the substrate water molecule via D1-Asp61 and electron transfer via redox-active D1-Tyr161 (TyrZ) to the chlorophyll pair in Cl--depleted PSII using a quantum mechanical/molecular mechanical approach. The low-barrier H-bond formation between the substrate water molecule and D1-Asp61 remained unaffected upon the depletion of Cl-. However, the binding site, D2-Lys317, formed a salt bridge with D1-Asp61, leading to the inhibition of the subsequent proton transfer. Remarkably, the redox potential (Em) of S2/S3 increased significantly, making electron transfer from S2 to TyrZ energetically uphill, as observed in Ca2+-depleted PSII. The uphill electron transfer pathway was induced by the significant increase in Em(S2/S3) caused by the loss of charge compensation for D2-Lys317 upon the depletion of Cl-, whereas it was induced by the significant decrease in Em(TyrZ) caused by the rearrangement of the water molecules at the Ca2+ binding moiety upon the depletion of Ca2+." @default.
- W4200311938 created "2021-12-31" @default.
- W4200311938 creator A5023470018 @default.
- W4200311938 creator A5075044495 @default.
- W4200311938 creator A5079397709 @default.
- W4200311938 date "2021-12-25" @default.
- W4200311938 modified "2023-10-16" @default.
- W4200311938 title "Requirement of Chloride for the Downhill Electron Transfer Pathway from the Water-Splitting Center in Natural Photosynthesis" @default.
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- W4200311938 doi "https://doi.org/10.1021/acs.jpcb.1c09176" @default.
- W4200311938 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/34955014" @default.
- W4200311938 hasPublicationYear "2021" @default.