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A new tri-nuclear Cu-carbonate cluster utilizing CO2 as a C1-building block - reactive intermediates, a probable mechanism, and EPR and magnetic studies
Univ New South Wales, Sch Chem, Sydney, NSW 2052, Australia.ORCID iD: 0000-0003-1256-501X
Univ New South Wales, Mark Wainwright Analyt Ctr, Sydney, NSW 2052, Australia.ORCID iD: 0000-0003-3693-9063
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. (Syntetisk molekylkemi)ORCID iD: 0000-0001-7643-302X
Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia.ORCID iD: 0000-0003-2205-3106
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2019 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 48, no 11, p. 3576-3582Article in journal (Refereed) Published
Abstract [en]

This work demonstrates that simple copper-bipyridine compounds and atmospheric CO2 react to produce useful/complex materials under appropriate conditions. Starting from a distorted square planar copper(II) complex, [((tbu)bpy)CuCl2]((tbu)bpy = 4-tert-butyl-2-(4-tert-butylpyridin-2-yl)pyridine), an air-sensitive, copper(I) complex,[((tbu)bpy)(2)Cu-I][BF4], which exhibits a distorted tetrahedral geometry, was synthesized and characterized. Reactions of [((tbu)bpy)(2)Cu-I][BF4] with CO2 inside a sealed tube and with air were carried out over a week and three weeks, respectively. A new tricopper(II)-carbonato cluster, [{((tbu)bpy)(2)Cu}(3)(mu-CO3)][PF6](4), was isolated with three distorted octahedral copper(II) centres bound by a carbonate-bridge formed from atmospheric CO2. NMR and UV-Vis spectroscopic analyses coupled with previous reports point to a multi-step process in the formation of a trinuclear Cu-II-carbonato cluster that includes the probable involvement of mu-hydroxo-bridged dicopper(II) type intermediates.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2019. Vol. 48, no 11, p. 3576-3582
National Category
Inorganic Chemistry Physical Chemistry
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URN: urn:nbn:se:uu:diva-380436DOI: 10.1039/c8dt04858dISI: 000461088700031PubMedID: 30741285OAI: oai:DiVA.org:uu-380436DiVA, id: diva2:1300751
Funder
Australian Research Council, DP 160104383Available from: 2019-03-29 Created: 2019-03-29 Last updated: 2019-03-29Bibliographically approved

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Thapper, Anders

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Das, BiswanathBhadbhade, MohanThapper, AndersLing, Chris D.
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