ArticleJournal of the American Chemical Society2013
Enhanced electron-transfer reactivity of nonheme manganese(IV)-oxo complexes by binding scandium ions.
Article in Journal of the American Chemical Society, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. An erratum has been issued. Cited by 30 papers.
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30 citing papers in PubMed, 150 citations in OpenAlex.
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Corrections and comments
- Erratum issuedFuhkuzumi, Shunichi [corrected to Fukuzumi, Shunichi]
Authors and funding
8 authors at 3 institutions in 3 countries.
Funding
Abstract
One and two scandium ions (Sc(3+)) are bound strongly to nonheme manganese(IV)-oxo complexes, [(N4Py)Mn(IV)(O)](2+) (N4Py = N,N-bis(2-pyridylmethyl)-N-bis(2-pyridyl)methylamine) and [(Bn-TPEN)Mn(IV)(O)](2+) (Bn-TPEN = N-benzyl-N,N',N'-tris(2-pyridylmethyl)-1,2-diaminoethane), to form Mn(IV)(O)-(Sc(3+))1 and Mn(IV)(O)-(Sc(3+))2 complexes, respectively. The binding of Sc(3+) ions to the Mn(IV)(O) complexes was examined by spectroscopic methods as well as by DFT calculations. The one-electron reduction potentials of the Mn(IV)(O) complexes were markedly shifted to a positive direction by binding of Sc(3+) ions. Accordingly, rates of the electron transfer reactions of the Mn(IV)(O) complexes were enhanced as much as 10(7)-fold by binding of two Sc(3+) ions. The driving force dependence of electron transfer from various electron donors to the Mn(IV)(O) and Mn(IV)(O)-(Sc(3+))2 complexes was examined and analyzed in light of the Marcus theory of electron transfer to determine the reorganization energies of electron transfer. The smaller reorganization energies and much more positive reduction potentials of the Mn(IV)(O)-(Sc(3+))2 complexes resulted in remarkable enhancement of the electron-transfer reactivity of the Mn(IV)(O) complexes. Such a dramatic enhancement of the electron-transfer reactivity of the Mn(IV)(O) complexes by binding of Sc(3+) ions resulted in the change of mechanism in the sulfoxidation of thioanisoles by Mn(IV)(O) complexes from a direct oxygen atom transfer pathway without metal ion binding to an electron-transfer pathway with binding of Sc(3+) ions.
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