Redox-inactive metal ions modulate the reactivity and oxygen release of mononuclear non-haem iron(III)-peroxo complexes
- Authors
- Bang, S (Bang, Suhee); Lee, YM (Lee, Yong-Min); Hong, S (Hong, Seungwoo); Cho, KB (Cho, Kyung-Bin); Nishida, Y (Nishida, Yusuke); Seo, MS (Seo, Mi Sook); Sarangi, R (Sarangi, Ritimukta; Fukuzumi, S (Fukuzumi, Shunich; Nam, W (Nam, Wonwoo)
- Issue Date
- Oct-2014
- Publisher
- NATURE PUBLISHING GROUP
- Citation
- NATURE CHEMISTRY, v.6, no.10, pp 934 - 940
- Pages
- 7
- Journal Title
- NATURE CHEMISTRY
- Volume
- 6
- Number
- 10
- Start Page
- 934
- End Page
- 940
- URI
- https://scholarworks.sookmyung.ac.kr/handle/2020.sw.sookmyung/147256
- DOI
- 10.1038/nchem.2055
- ISSN
- 1755-4330
1755-4349
- Abstract
- 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-(mu,eta(2):eta(2)-O-2)-Mn+ (Mn+ = Sr2+, Ca2+, Zn2+, Lu3+, Y3+ and Sc3+; TMC, 1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane). We demonstrate that the Ca2+ and Sr2+ 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 Ca2+ or Sr2+ 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 Ca2+ ion in the oxidation of water to dioxygen by the oxygen-evolving complex.
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