Modulation of multimetal complexation behavior of tetraoxime ligand by covalent transformation of olefinic functionalities

Inorganic Chemistry
Shigehisa AkineTatsuya Nabeshima

Abstract

A new multimetal complexation system that can change its complexation behavior by C-C bond formation has been developed. The acyclic tetraoxime ligand H(4)L(1) having two terminal allyl groups was synthesized. The olefin metathesis of H(4)L(1) selectively produced trans-H(4)L(2) while the reaction of [L(1)Zn(2)Ca] exclusively afforded cis-H(4)L(2). The saturated analogue H(4)L(3) was synthesized by hydrogenation. The complexation of the ligands H(4)L (L = L(1), trans-L(2), cis-L(2), L(3)) with zinc(II) acetate (3 equiv) yielded the trinuclear complexes [LZn(3)] with a similar trinuclear core bridged by acetato ligands. Whereas the formation process of [L(1)Zn(3)] having an acyclic ligand was highly cooperative, the macrocyclic analogues [LZn(3)] (L = trans-L(2), cis-L(2), L(3)) were formed in a stepwise fashion via the intermediate 2:3 complex [(HL)(2)Zn(3)]. The trinuclear complexes [LZn(3)] (L = L(1), trans-L(2), cis-L(2), L(3)) can recognize alkaline earth metal ions via site-selective metal exchange. The acyclic [L(1)Zn(3)] selectively recognizes Ca(2+), while the cyclic [trans-L(2)Zn(3)] showed a Ba(2+) selectivity. The metal exchange of [LZn(3)] (L = L(1), trans-L(2), cis-L(2), L(3)) with La(3+) efficiently occurred to gi...Continue Reading

References

Feb 15, 2001·Accounts of Chemical Research·T M Trnka, R H Grubbs
Jan 18, 2003·Angewandte Chemie·Aleksey V ChuchuryukinGerard van Koten
Jan 13, 2005·Journal of the American Chemical Society·Shigehisa AkineTatsuya Nabeshima
Jan 22, 2005·Angewandte Chemie·Xiaowu Yang, Bing Gong
Jan 5, 2006·Journal of the American Chemical Society·Mark S KaucherJeffery T Davis
Dec 7, 2006·Journal of the American Chemical Society·Shigehisa AkineTatsuya Nabeshima
May 1, 2007·Chemistry : a European Journal·Olena MolokanovaVolker Böhmer
Mar 29, 2008·Inorganic Chemistry·Shigehisa AkineTatsuya Nabeshima
Aug 4, 2009·Journal of the American Chemical Society·Shuichi HiraokaMitsuhiko Shionoya

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Citations

Oct 18, 2011·Chemistry : a European Journal·Elena TulyakovaOlga Fedorova
Apr 12, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Ryan M Clarke, Tim Storr
Aug 19, 2015·Acta Crystallographica. Section E, Crystallographic Communications·Józef UtkoTadeusz Lis
May 5, 2011·Chemistry : a European Journal·Shigehisa AkineTatsuya Nabeshima

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