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• W3025172790 endingPage "10704" @default.
• W3025172790 startingPage "10692" @default.
• W3025172790 abstract "Valence tautomerism (VT) involves a reversible stimulated intramolecular electron transfer between a redox-active ligand and redox-active metal. Bis(dioxolene)-bridged dinuclear cobalt compounds provide an avenue toward controlled two-step VT interconversions of the form {CoIII-cat-cat-CoIII} ⇌ {CoIII-cat-SQ-CoII}⇌{CoII-SQ-SQ-CoII} (cat2– = catecholate, SQ•– = semiquinonate). Design flexibility for dinuclear VT complexes confers an advantage over two-step spin crossover complexes for future applications in devices or materials. The four dinuclear cobalt complexes in this study are bridged by deprotonated 3,3,3′,3′-tetramethyl-1,1′-spirobi(indan)-5,5′,6,6′-tetraol (spiroH4) or 3,3,3′,3′-tetramethyl-1,1′-spirobi(indan)-4,4′,7,7′-tetrabromo-5,5′,6,6′-tetraol (Br4spiroH4) with Mentpa ancillary ligands (tpa = tris(2-pyridylmethyl)amine, n = 0–3 corresponds to methylation of the 6-position of the pyridine rings). Complementary structural, magnetic, spectroscopic, and density functional theory (DFT) computational studies reveal different electronic structures and VT behavior for the four cobalt complexes; one-step one-electron partial VT, two-step VT, incomplete VT, and temperature-invariant {CoIII-cat-cat-CoIII} states are observed. Electrochemistry, DFT calculations, and the study of a mixed-valence {ZnII-cat-SQ-ZnII} analog have allowed elucidation of thermodynamic parameters governing the one- and two-step VT behavior. The VT transition profile is rationalized by (1) the degree of electronic communication within the bis(dioxolene) ligand and (2) the matching of cobalt and dioxolene redox potentials. This work establishes a clear path to the next generation of two-step VT complexes through incorporation of mixed-valence class II and class II-III bis(dioxolene) bridging ligands with sufficiently weak intramolecular coupling." @default.
• W3025172790 created "2020-05-21" @default.
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• W3025172790 date "2020-05-15" @default.
• W3025172790 modified "2023-10-16" @default.
• W3025172790 title "Understanding the Origin of One- or Two-Step Valence Tautomeric Transitions in Bis(dioxolene)-Bridged Dinuclear Cobalt Complexes" @default.
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• W3025172790 doi "https://doi.org/10.1021/jacs.0c01073" @default.
• W3025172790 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/32412246" @default.
• W3025172790 hasPublicationYear "2020" @default.
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