ArticleInorganic chemistry2013
Synthetic cluster models of biological and heterogeneous manganese catalysts for O2 evolution.
Article in Inorganic chemistry, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 34 papers.
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34 citing papers in PubMed, 139 citations in OpenAlex.
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- Spectroscopic and Theoretical Investigation of Water Binding in a Copper-Calcium Complex.The journal of physical chemistry. A · 2025Article
- Cluster dynamics of heterometallic trinuclear clusters during ligand substitution, redox chemistry, and group transfer processes.Chemical science · 2024Article
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- Redox Processes Involving Oxygen: The Surprising Influence of Redox-Inactive Lewis Acids.JACS Au · 2024Review
- Comparative Density Functional Theory Study of Magnetic Exchange Couplings in Dinuclear Transition-Metal Complexes.Journal of chemical theory and computation · 2023Article
- Coordination Number in High-Spin-Low-Spin Equilibrium in Cluster Models of the SJournal of the American Chemical Society · 2023Article
- MnInorganic chemistry · 2023Article
- Mimicking the Oxygen-Evolving Center in Photosynthesis.Frontiers in plant science · 2022Review
- De novo metalloprotein design.Nature reviews. Chemistry · 2022Article
- Structural dynamics in the water and proton channels of photosystem II during the SNature communications · 2021Article
- Article
- CaMnAngewandte Chemie (International ed. in English) · 2021Article
- Effects of Noncovalent Interactions on High-Spin Fe(IV)-Oxido Complexes.Journal of the American Chemical Society · 2020Article
- Article
- Effects of Lewis Acidic Metal Ions (M) on Oxygen-Atom Transfer Reactivity of Heterometallic MnInorganic chemistry · 2019Article
- Tetranuclear [MnJournal of the American Chemical Society · 2018Article
- Thermodynamics of Proton and Electron Transfer in Tetranuclear Clusters with Mn-OHJournal of the American Chemical Society · 2018Article
- Intramolecular C-H and C-F Bond Oxygenation by Site-Differentiated Tetranuclear Manganese Models of the OEC.Inorganic chemistry · 2017Article
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3 authors at 1 institution in 1 country.
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Abstract
Artificial photosynthesis has emerged as an important strategy toward clean and renewable fuels. Catalytic oxidation of water to O2 remains a significant challenge in this context. A mechanistic understanding of currently known heterogeneous and biological catalysts at a molecular level is highly desirable for fundamental reasons as well as for the rational design of practical catalysts. This Award Article discusses recent efforts in synthesizing structural models of the oxygen-evolving complex of photosystem II. These structural motifs are also related to heterogeneous mixed-metal oxide catalysts. A stepwise synthetic methodology was developed toward achieving the structural complexity of the targeted active sites. A geometrically restricted multinucleating ligand, but with labile coordination modes, was employed for the synthesis of low-oxidation-state trimetallic species. These precursors were elaborated to site-differentiated tetrametallic complexes in high oxidation states. This methodology has allowed for structure-reactivity studies that have offered insight into the effects of different components of the clusters. Mechanistic aspects of oxygen-atom transfer and incorporation from water have been interrogated. Significantly, a large and systematic effect of redox-inactive metals on the redox properties of these clusters was discovered. With the pKa value of the redox-inactive metal-aqua complex as a measure of the Lewis acidity, structurally analogous clusters display a linear dependence between the reduction potential and acidity; each pKa unit shifts the potential by ca. 90 mV. Implications for the function of the biological and heterogeneous catalysts are discussed.
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