Towards an artificial model for Photosystem II: a manganese(II,II) dimer covalently linked to ruthenium(II) tris-bipyridine via a tyrosine derivative

Sun, Licheng; Raymond, Mary Katherine; Magnuson, Ann; LeGourriérec, Denis; Tamm, Marcus; Abrahamsson, Malin; Kenéz, Ping Huang; Mårtensson, Jerker; Stenhagen, Gunnar; Hammarström, Leif; Styring, Stenbjörn; Åkermark, Björn

doi:10.1016/s0162-0134(99)00200-7

Cited by 72 publications

(27 citation statements)

References 31 publications

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“… 45 − 48 Models for Tyr radical formation have also been developed and coupled to a Mn cluster similar to the water-oxidizing complex (WOC). 39 − 42 , 49 , 50 …”

Section: Tyrosyl Radical Environmentsmentioning

confidence: 99%

Biochemistry and Theory of Proton-Coupled Electron Transfer

et al. 2014

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havior in PCET 3400 5.3. Adiabatic and Nonadiabatic PCET Interpreted in the Context of the Schrodinger Equation and the Born−Oppenheimer (Adiabatic) Approximation 3404 5.3.1. Quantum-State Dynamics of PCET Systems and the Underlying Potential (Free) Energy Surfaces 3404 5.3.2. Investigating Coupled Electronic−Nuclear Dynamics and Deviations from the Adiabatic Approximation in PCET Systems via a Simple Model 3408 5.3.3. Formulation and Representations of Electron−Proton States 6. Extension of Marcus Theory to Proton and Atom Transfer Reactions 6.1. Extended Marcus Theory for Electron, Proton, and Atom Transfer Reactions 6.2. Implications of the Extended Marcus Theory: Brønsted Slope, Kinetic Isotope Effect, and Cross-Relation 7. Beyond Marcus Theory: Nuclear Tunneling and Structural Constraints on PCET 8. Proton-Activated Electron Transfer: A Special Case of Separable and Coupled PT and ET 9. Dogonadze−Kuznetsov−Levich (DKL) Model of PT/HAT and Connections with ET and PCET Theories 10. Borgis−Hynes (BH) Theory for PT and HAT 10.1. Dynamical Regimes of the BH Theory 10.2. Splitting and Coupling Fluctuations 10.3. Reaction Rate Constant 10.4. Analytical Rate Constant Expressions in Limiting Regimes 11. Cukier Theory of PCET 11.1. Double-Adiabatic and Two-Dimensional Approaches 11.2. Reorganization and Solvation Free Energy in ET, PT, and EPT 11.3. Generalization of the Theory and Connections between PT, PCET, and HAT 12. Soudackov−Hammes-Schiffer (SHS) Theory of PCET 12.1. Regarding System Coordinates and Interactions: Hamiltonians and Free Energies 12.2. Electron−Proton States, Rate Constants, and Dynamical Effects 12.3. Note on the Kinetic Isotope Effect in PCET 12.4. Distinguishing between HAT and Concerted PCET Reactions 12.5. Electrochemical PCET 13. Conclusions and Prospects Appendix A Appendix B Associated Content Supporting Information

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“… 45 − 48 Models for Tyr radical formation have also been developed and coupled to a Mn cluster similar to the water-oxidizing complex (WOC). 39 − 42 , 49 , 50 …”

Section: Tyrosyl Radical Environmentsmentioning

confidence: 99%

Biochemistry and Theory of Proton-Coupled Electron Transfer

et al. 2014

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“…In a comparable approach, the groups of Åkermark, Hammarström, and Styring have studied a dinuclear manganese system based on the bpmp (bpmp = 2,6-bis[[N,N-di(2-pyridylmethyl)amino]methyl]-4-methylphenol) ligand with a ruthenium-polypyridyl sensitizer linked through covalent modification of the 4-positions on polypyridyl and phenolate ligands [175, 176]. The manganese dimer, shown in Figure 17, can be oxidized from Mn III /Mn III to Mn III /Mn IV , demonstrating that advancement of the oxidation state is possible, even if catalytic turnover is not.…”

Section: Catalysis For Light-driven Water Oxidationmentioning

confidence: 99%

Light-driven water oxidation for solar fuels

Young

Martini

Milot

et al. 2012

Coordination Chemistry Reviews

353

314

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Light-driven water oxidation is an essential step for conversion of sunlight into storable chemical fuels. Fujishima and Honda reported the first example of photoelectrochemical water oxidation in 1972. In their system, TiO2 was irradiated with ultraviolet light, producing oxygen at the anode and hydrogen at a platinum cathode. Inspired by this system, more recent work has focused on functionalizing nanoporous TiO2 or other semiconductor surfaces with molecular adsorbates, including chromophores and catalysts that absorb visible light and generate electricity (i.e., dye-sensitized solar cells) or trigger water oxidation at low overpotentials (i.e., photocatalytic cells). The physics involved in harnessing multiple photochemical events for multielectron reactions, as required in the four-electron water oxidation process, has been the subject of much experimental and computational study. In spite of significant advances with regard to individual components, the development of highly efficient photocatalytic cells for solar water splitting remains an outstanding challenge. This article reviews recent progress in the field with emphasis on water-oxidation photoanodes inspired by the design of functionalized thin film semiconductors of typical dye-sensitized solar cells.

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“…(ii) Competing kinetics in accumulative electron transfer The excited state of the Ru unit of the Ru-Mn 2 (II,II) complex in figure 2 has a lifetime of 110 ns (Sun et al 2000). This allows efficient electron transfer to an acceptor to generate the Ru 3C state, and subsequent oxidation of the manganese dimer.…”

Section: Resultsmentioning

confidence: 99%

Coupled electron transfers in artificial photosynthesis

Hammarström

Styring

2007

Phil. Trans. R. Soc. B

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Light-induced charge separation in molecular assemblies has been widely investigated in the context of artificial photosynthesis. Important progress has been made in the fundamental understanding of electron and energy transfer and in stabilizing charge separation by multi-step electron transfer. In the Swedish Consortium for Artificial Photosynthesis, we build on principles from the natural enzyme photosystem II and Fe-hydrogenases. An important theme in this biomimetic effort is that of coupled electron-transfer reactions, which have so far received only little attention. (i) Each absorbed photon leads to charge separation on a single-electron level only, while catalytic water splitting and hydrogen production are multi-electron processes; thus there is the need for controlling accumulative electron transfer on molecular components. (ii) Water splitting and proton reduction at the potential catalysts necessarily require the management of proton release and/or uptake. Far from being just a stoichiometric requirement, this controls the electron transfer processes by proton-coupled electron transfer (PCET). (iii) Redox-active links between the photosensitizers and the catalysts are required to rectify the accumulative electron-transfer reactions, and will often be the starting points of PCET.

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Towards an artificial model for Photosystem II: a manganese(II,II) dimer covalently linked to ruthenium(II) tris-bipyridine via a tyrosine derivative

Cited by 72 publications

References 31 publications

Biochemistry and Theory of Proton-Coupled Electron Transfer

Biochemistry and Theory of Proton-Coupled Electron Transfer

Light-driven water oxidation for solar fuels

Coupled electron transfers in artificial photosynthesis

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