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Redox-inactive metal ions modulate the reactivity and oxygen release of mononuclear non-haem iron(III)–peroxo complexes
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Redox-inactive metal ions modulate the reactivity and oxygen release of mononuclear non-haem iron(III)–peroxo complexes
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Journal Article
Redox-inactive metal ions modulate the reactivity and oxygen release of mononuclear non-haem iron(III)–peroxo complexes
2014
Overview
Redox-inactive metal ions that function as Lewis acids play pivotal roles in modulating the reactivity of oxygen-containing metal complexes and metalloenzymes, such as the oxygen-evolving complex in photosystem II and its small-molecule mimics. Here we report the synthesis and characterization of non-haem iron(
III
)–peroxo complexes that bind redox-inactive metal ions, (TMC)Fe
III
–(μ,η
2
:η
2
-O
2
)–M
n
+
(M
n
+
= Sr
2+
, Ca
2+
, Zn
2+
, Lu
3+
, Y
3+
and Sc
3+
; TMC, 1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane). We demonstrate that the Ca
2+
and Sr
2+
complexes showed similar electrochemical properties and reactivities in one-electron oxidation or reduction reactions. However, the properties and reactivities of complexes formed with stronger Lewis acidities were found to be markedly different. Complexes that contain Ca
2+
or Sr
2+
ions were oxidized by an electron acceptor to release O
2
, whereas the release of O
2
did not occur for complexes that bind stronger Lewis acids. We discuss these results in the light of the functional role of the Ca
2+
ion in the oxidation of water to dioxygen by the oxygen-evolving complex.
Non-haem iron(
III
)-peroxo complexes that bind redox-inactive metal ions are synthesized to investigate the role of the Ca
2+
ion in the oxidation of water to dioxygen in photosystem II. The electrochemical properties and reactions of these compounds with an electron donor and an acceptor are found to be markedly dependent on the Lewis acidity of redox-inactive metal ions.
Publisher
Nature Publishing Group UK,Nature Publishing Group
