Probing Redox Noninnocence of Copper and Zinc Bis‐pyridylpyrrolides

Flores, Jaime A.; Andino, José G.; Lord, Richard L.; Wolfe, Robert J.; Park, Hyunsoo; Pink, Maren; Telser, Joshua; Caulton, Kenneth G.

doi:10.1002/ejic.201800935

Title: Probing Redox Noninnocence of Copper and Zinc Bis‐pyridylpyrrolides

Journal Article · Wed Nov 28 00:00:00 EST 2018 · European Journal of Inorganic Chemistry

DOI:https://doi.org/10.1002/ejic.201800935· OSTI ID:1483730

Flores, Jaime A. ^[1]; Andino, José G. ^[1];

^[2]; Wolfe, Robert J. ^[1];

^[1];

^[3];

^[1]

Department of Chemistry Indiana University 800 East Kirkwood Avenue 47405 USA Bloomington Indiana47405 USA
Department of Chemistry Grand Valley State University 49401 Allendale Michigan USA
Department of Biological Physical and Health Sciences Roosevelt University 430 South Michigan Avenue 60605 Chicago Illinois USA

A series of complexes of divalent copper and zinc carrying two systematically substituted 2,2′‐pyridylpyrrolide ligands, designated L ⁿ to indicate the number of pyrrole CF ₃ substituents ( n = 0, 1, 2), have been studied for their geometric and electronic structures. These reveal the pyridylpyrrolide to be a highly anisotropic nitrogen donor ligand which distorts ML ₂ complexes away from both planar and tetrahedral structures. Characterization includes CV and mass spectrometry, which show access to cations beyond conventional maximum metal oxidation states. EPR studies at multiple microwave frequencies of the series Cu(L ⁿ ) ₂ gave insight into the substituent effect on frontier orbital composition of these complexes. While Cu(L ² ) ₂ exhibited EPR spectra that were roughly comparable to those for typical, tetragonally distorted Cu ^II complexes with the SOMO having d _x ² _– _y ² character, the other two complexes exhibited more unusual EPR spectra indicative of their distinct geometry, reminiscent of equatorially‐vacant trigonal bipyramidal hybridization and fully consistent with the X‐ray crystal structure determinations of all three Cu(L ⁿ ) ₂ . DFT calculations map both geometric and delocalization changes upon redox change, and show the relevance of oxidation at the pyrrolide donors rather than at the metal.

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Sponsoring Organization:: USDOE

OSTI ID:: 1483730

Journal Information:: European Journal of Inorganic Chemistry, Journal Name: European Journal of Inorganic Chemistry Vol. 2018 Journal Issue: 45; ISSN 1434-1948

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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