Linked Life Data

19230704

Source:http://linkedlifedata.com/resource/pubmed/id/19230704

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pubmed-article:19230704pubmed:dateCreated2009-5-18lld:pubmed
pubmed-article:19230704pubmed:abstractTextThe dissociation of [Cu(II)(L)His](*2+) complexes [L = diethylenetriamine (dien) or 1,4,7-triazacyclononane (9-aneN(3))] bears a strong resemblance to the previously reported behavior of [Cu(II)(L)GGH](*2+) complexes. We have used low-energy collision-induced dissociation experiments and density functional theory (DFT) calculations at the B3LYP/6-31+G(d) level to study the macrocyclic effect of the auxiliary ligands on the formation of His(*+) from prototypical [Cu(II)(L)His](*2+) systems. DFT revealed that the relative energy barriers of the same electron-transfer (ET) dissociation pathways of [Cu(II)(9-aneN(3))His](*2+) and [Cu(II)(dien)His](*2+) are very similar, with the ET reactions of [Cu(II)(9-aneN(3))His](*2+) leading to the generation of two distinct His(*+) species; in contrast, the proton transfer (PT) dissociation pathways of [Cu(II)(9-aneN(3))His](*2+) and [Cu(II)(dien)His](*2+) differ considerably. The PT reactions of [Cu(II)(9-aneN(3))His](*2+) are associated with substantially higher barriers (>13 kcal/mol) than those of [Cu(II)(dien)His](*2+). Thus, the sterically encumbered auxiliary 9-aneN(3) ligand facilitates ET reactions while moderating PT reactions, allowing the formation of hitherto nonobservable histidine radical cations.lld:pubmed
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pubmed-article:19230704pubmed:year2009lld:pubmed
pubmed-article:19230704pubmed:articleTitleExperimental and computational studies of the macrocyclic effect of an auxiliary ligand on electron and proton transfers within ternary copper(II)-histidine complexes.lld:pubmed
pubmed-article:19230704pubmed:affiliationDepartment of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong, China.lld:pubmed
pubmed-article:19230704pubmed:publicationTypeJournal Articlelld:pubmed
pubmed-article:19230704pubmed:publicationTypeResearch Support, U.S. Gov't, Non-P.H.S.lld:pubmed
pubmed-article:19230704pubmed:publicationTypeResearch Support, Non-U.S. Gov'tlld:pubmed