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Heteronuclear assembly of Ni–Cu dithiolato complexes: synthesis, structures, and reactivity studies

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Abstract

Heterometallic complexes exhibit the advantages of exceptional crystal structures and electronic performance over monometallic ones in mimicking the active site of metalloenzymes such as [NiFe] hydrogenase and acetyl-coenzyme A synthase/carbon monoxide dehydrogenase (ACS/CODH). Herein, we discovered a new mild route to synthesize [NiCu] binuclear complexes [(dppe)Ni(μ-pdt)Cu(dppe)](BF4) (dppe = 1,2-C2H4(PPh2)2, 1), [(dppe)Ni(μ-pdt)Cu(dppbz)]BF4 (dppbz = 1,2-C6H4(PPh2)2; 2), and [(dppe)Ni(μ-pdt)Cu(dcpe)]BF4 (dcpe = 1,2-C2H4(PCy2)2; 3) through Ni(pdt)(dppe) (pdt = (SC3H6S)2−) and [Cu(P–P)(NCMe)2]BF4 (P–P = diphosphine chelating ligand). The structures of these models in the [(dppe)Ni(pdt)Cu(P–P)]+ type are composed of Cu(I) in tetrahedral and Ni(II) in planar conformations. DFT calculations suggest that the HOMO corresponds to the delocalized π-orbital of the P–Cu–S system, while the LUMO is primarily composed of Ni, P, and S atoms with antibonding character.

Graphical abstract: Heteronuclear assembly of Ni–Cu dithiolato complexes: synthesis, structures, and reactivity studies

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Publication details

The article was received on 28 Nov 2016, accepted on 25 Jan 2017, published on 07 Feb 2017 and first published online on 07 Feb 2017


Article type: Research Article
DOI: 10.1039/C6QI00536E
Citation: Inorg. Chem. Front., 2017, Advance Article
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    Heteronuclear assembly of Ni–Cu dithiolato complexes: synthesis, structures, and reactivity studies

    X. Chu, X. Xu, H. Su, S. Raje, R. Angamuthu, C. Tung and W. Wang, Inorg. Chem. Front., 2017, Advance Article , DOI: 10.1039/C6QI00536E

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