A series of peroxomanganese(III) complexes supported by tetradentate aminopyridyl ligands: detailed spectroscopic and computational studies

Journal of the American Chemical Society
Robert A GeigerTimothy A Jackson

Abstract

A set of four [Mn(II)(L(7)py(2)(R))](2+) complexes, supported by the tetradentate 1,4-bis(2-pyridylmethyl)-1,4-diazepane ligand and derivatives with pyridine substituents in the 5 (R = Br) and 6 positions (R = Me and MeO), are reported. X-ray crystal structures of these complexes all show the L(7)py(2)(R) ligands bound to give a trans complex. Treatment of these Mn(II) precursors with either H(2)O(2)/Et(3)N or KO(2) in MeCN at -40 degrees C results in the formation of peroxomanganese complexes [Mn(III)(O(2))(L(7)py(2)(R))](+) differing only in the identity of the pyridine ring substituent. The electronic structures of two of these complexes, [Mn(III)(O(2))(L(7)py(2)(H))](+) and [Mn(III)(O(2))(L(7)py(2)(Me))](+), were examined in detail using electronic absorption, low-temperature magnetic circular dichroism (MCD) and variable-temperature variable-field (VTVH) MCD spectroscopies to determine ground-state zero-field splitting (ZFS) parameters and electronic transition energies, intensities, and polarizations. DFT and TD-DFT computations were used to validate the structures of [Mn(III)(O(2))(L(7)py(2)(H))](+) and [Mn(III)(O(2))(L(7)py(2)(Me))](+), further corroborating their assignment as peroxomanganese(III) species. While these ...Continue Reading

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Citations

Nov 28, 2013·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Domenick F Leto, Timothy A Jackson
Jul 23, 2011·Journal of the American Chemical Society·Michael K Coggins, Julie A Kovacs
Nov 3, 2016·Journal of the American Chemical Society·Shengfa YeFrank Neese
May 6, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Jisheng ZhangGuochuan Yin
Jun 1, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Junyi DuWei Sun
Jul 18, 2017·European Journal of Inorganic Chemistry·Hannah E ColmerJoshua Telser
Sep 6, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Melissa C DenlerTimothy A Jackson
Apr 4, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Chien-Ming LeeWonwoo Nam
Apr 11, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Hans-Martin BerendsPhilipp Kurz
Mar 29, 2014·Chemical Communications : Chem Comm·Michaela GrauGeorge J P Britovsek
Oct 15, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Hannah E ColmerTimothy A Jackson
May 22, 2013·Chemical Communications : Chem Comm·Sanae El GhachtouliElodie Anxolabéhère-Mallart
Jan 26, 2011·Dalton Transactions : an International Journal of Inorganic Chemistry·Robert A GeigerTimothy A Jackson
Nov 23, 2017·Angewandte Chemie·Adriana M MagherusanAidan R McDonald
Jan 9, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Rishi Kant, Suman Maji
Feb 4, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Dattaprasad D NarulkarSunder N Dhuri
Apr 15, 2021·Journal of the American Chemical Society·Alexandra N DowningJulie A Kovacs
Aug 15, 2014·Journal of the American Chemical Society·Hee SoWonwoo Nam
Apr 14, 2020·Inorganic Chemistry·Eva M ZolnhoferJoshua Telser
Sep 9, 2021·Journal of the American Chemical Society·Adedamola A OpaladeTimothy A Jackson
Nov 4, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Emma N Cook, Charles W Machan

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