2022
DOI: 10.21203/rs.3.rs-1210297/v1
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The electron-proton bottleneck of photosynthetic oxygen evolution

Abstract: Photosynthesis fuels life on Earth by storing solar energy in chemical form, inspiring technological schemes for sustainable fuel production. Today’s oxygen-rich atmosphere results from photosynthetic O2-production during water-splitting at the protein-bound manganese cluster of photosystem II. Formation of the O2 molecule starts from a state with four accumulated electron holes, the S4-state, postulated half a century ago1 and remaining enigmatic ever since. Here we resolve this missing key element in photosy… Show more

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Cited by 2 publications
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“…Three channel networks have been identified and variously named (Murray and Barber 2007 ; Ho and Styring 2008 ; Gabdulkhakov et al 2009 ; Guskov et al 2009 ; Vassiliev et al 2010 ; Umena et al 2011 ; Sakashita et al 2017a ). The Cl1 channel has been shown to be crucial for proton egress (Hussein et al 2021 ; Dau et al 2022 ), but also the O4 channel may have that function during the S 0 ⟶ S 1 transition (Sakashita et al 2017a ; Hussein et al 2021 ). All the three channels (Fig.…”
Section: Chemical Reactionsmentioning
confidence: 99%
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“…Three channel networks have been identified and variously named (Murray and Barber 2007 ; Ho and Styring 2008 ; Gabdulkhakov et al 2009 ; Guskov et al 2009 ; Vassiliev et al 2010 ; Umena et al 2011 ; Sakashita et al 2017a ). The Cl1 channel has been shown to be crucial for proton egress (Hussein et al 2021 ; Dau et al 2022 ), but also the O4 channel may have that function during the S 0 ⟶ S 1 transition (Sakashita et al 2017a ; Hussein et al 2021 ). All the three channels (Fig.…”
Section: Chemical Reactionsmentioning
confidence: 99%
“…Interestingly, the slow kinetic of the S 3 → S 4 → S 0 transition appears to be connected to large entropic contributions rather than a high activation barrier. This indicates that a large number of conformational states may need to be sampled to find the optimal configuration of the Mn 4 CaO 5 cluster and the H-bonding network to allow generation of the S 4 state as well as O 2 formation and release (Zaharieva and Dau 2019 ; Dau et al 2022 ). Lastly, the S 3 → S 4 → S 0 transition is irreversible due to its large driving force (Haumann et al 2008 ; Kolling et al 2009 ; Shevela et al 2011 ; Nilsson et al 2016 ).…”
Section: Chemical Reactionsmentioning
confidence: 99%