Dimer-of-dimers model for the oxygen-evolving complex of photosystem II. Synthesis and properties of MnIV4O5(terpy) 4(H2O)2](CIO4)6

Hongyu Chen; J. W. Faller; Robert H. Crabtree; Gary W. Brudvig

doi:10.1021/ja037389l

Dimer-of-dimers model for the oxygen-evolving complex of photosystem II. Synthesis and properties of Mn^IV₄O₅(terpy) ₄(H₂O)₂](CIO₄)₆

Hongyu Chen, J. W. Faller, Robert H. Crabtree, Gary W. Brudvig

Yale University

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118 Citations (Scopus)

Abstract

A dimer-of-dimers model compound for the oxygen-evolving complex of photosystem II, [{(H₂O)-(terpy)Mn^IV(μ-O) ₂Mn^IV(terpy)}₂(μ-O)](CIO₄) ₆ (terpy = 2,2′:6′,2″-terpyridine), has been prepared and characterized by X-ray crystallography and ESI-MS. Low pH was found to promote the disproportionation of [Mn^III/IV ₂O₂(terpy)₂(OH₂)₂] ³⁺ to Mn²⁺ and a Mn^IV/IV₂O ₂(terpy)₂ species; the latter complex slowly dimerizes to form the title complex. Protonation of a μ-oxo bridge is proposed to initiate the disproportionation, based on analogy with the [Mn ^III/IV₂O₂(bpy)₄]³⁺ system.

Original language	English
Pages (from-to)	7345-7349
Number of pages	5
Journal	Journal of the American Chemical Society
Volume	126
Issue number	23
DOIs	https://doi.org/10.1021/ja037389l
Publication status	Published - Jun 16 2004

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ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

Cite this

Chen, H., Faller, J. W., Crabtree, R. H., & Brudvig, G. W. (2004). Dimer-of-dimers model for the oxygen-evolving complex of photosystem II. Synthesis and properties of Mn^IV₄O₅(terpy) ₄(H₂O)₂](CIO₄)₆. Journal of the American Chemical Society, 126(23), 7345-7349. https://doi.org/10.1021/ja037389l

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title = "Dimer-of-dimers model for the oxygen-evolving complex of photosystem II. Synthesis and properties of MnIV4O5(terpy) 4(H2O)2](CIO4)6",

abstract = "A dimer-of-dimers model compound for the oxygen-evolving complex of photosystem II, [{(H2O)-(terpy)MnIV(μ-O) 2MnIV(terpy)}2(μ-O)](CIO4) 6 (terpy = 2,2′:6′,2″-terpyridine), has been prepared and characterized by X-ray crystallography and ESI-MS. Low pH was found to promote the disproportionation of [MnIII/IV 2O2(terpy)2(OH2)2] 3+ to Mn2+ and a MnIV/IV2O 2(terpy)2 species; the latter complex slowly dimerizes to form the title complex. Protonation of a μ-oxo bridge is proposed to initiate the disproportionation, based on analogy with the [Mn III/IV2O2(bpy)4]3+ system.",

author = "Hongyu Chen and Faller, {J. W.} and Crabtree, {Robert H.} and Brudvig, {Gary W.}",

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AU - Crabtree, Robert H.

AU - Brudvig, Gary W.

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N2 - A dimer-of-dimers model compound for the oxygen-evolving complex of photosystem II, [{(H2O)-(terpy)MnIV(μ-O) 2MnIV(terpy)}2(μ-O)](CIO4) 6 (terpy = 2,2′:6′,2″-terpyridine), has been prepared and characterized by X-ray crystallography and ESI-MS. Low pH was found to promote the disproportionation of [MnIII/IV 2O2(terpy)2(OH2)2] 3+ to Mn2+ and a MnIV/IV2O 2(terpy)2 species; the latter complex slowly dimerizes to form the title complex. Protonation of a μ-oxo bridge is proposed to initiate the disproportionation, based on analogy with the [Mn III/IV2O2(bpy)4]3+ system.

AB - A dimer-of-dimers model compound for the oxygen-evolving complex of photosystem II, [{(H2O)-(terpy)MnIV(μ-O) 2MnIV(terpy)}2(μ-O)](CIO4) 6 (terpy = 2,2′:6′,2″-terpyridine), has been prepared and characterized by X-ray crystallography and ESI-MS. Low pH was found to promote the disproportionation of [MnIII/IV 2O2(terpy)2(OH2)2] 3+ to Mn2+ and a MnIV/IV2O 2(terpy)2 species; the latter complex slowly dimerizes to form the title complex. Protonation of a μ-oxo bridge is proposed to initiate the disproportionation, based on analogy with the [Mn III/IV2O2(bpy)4]3+ system.

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