Ancillary ligand control of electronic structure in o-benzoquinonediimine-ruthenium complex redox series: structures, electron paramagnetic resonance (EPR), and ultraviolet-visible-near-infrared (UV-vis-NIR) spectroelectrochemistry

Inorganic Chemistry
Ankita DasGoutam Kumar Lahiri

Abstract

The compounds Ru(acac)2(Q) (1), [Ru(bpy)2(Q)](ClO4)2 ([2](ClO4)2), and [Ru(pap)2(Q)]PF6 ([3]PF6), containing Q = N,N'-diphenyl-o-benzoquinonediimine and donating 2,4-pentanedionate ligands (acac(-)), π-accepting 2,2(/)-bipyridine (bpy), or strongly π-accepting 2-phenylazopyridine (pap) were prepared and structurally identified. The electronic structures of the complexes and several accessible oxidized and reduced forms were studied experimentally (electrochemistry, magnetic resonance, ultraviolet-visible-near-infrared (UV-vis-NIR) spectroelectrochemistry) and computationally (DFT/TD-DFT) to reveal significantly variable electron transfer behavior and charge distribution. While the redox system 1(+)-1(-) prefers trivalent ruthenium with corresponding oxidation states Q(0)-Q(2-) of the noninnocent ligand, the series 2(2+)-2(0) and 3(2+)-3(-) retain Ru(II). The bpy and pap co-ligands are not only spectators but can also be reduced prior to a second reduction of Q. The present study with new experimental and computational evidence on the influence of co-ligands on the metal is complementary to a report on the substituent effects in o-quinonediimine ligands [Kalinina et al., Inorg. Chem. 2008, 47, 10110] and to the discussion of the...Continue Reading

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Jan 11, 2013·Dalton Transactions : an International Journal of Inorganic Chemistry·Hemlata AgarwalaGoutam Kumar Lahiri
Aug 3, 2013·Dalton Transactions : an International Journal of Inorganic Chemistry·Ankita DasGoutam Kumar Lahiri
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Citations

Aug 6, 2015·Inorganic Chemistry·Abhishek MandalGoutam Kumar Lahiri
Feb 17, 2017·Inorganic Chemistry·Arijit Singha HazariGoutam Kumar Lahiri
Mar 16, 2017·Journal of the American Chemical Society·Benjamin R GarrettYiying Wu
Jun 27, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Ankita DasGoutam Kumar Lahiri
Jan 7, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Ankita DasGoutam Kumar Lahiri
Feb 20, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Prabir Ghosh, Goutam Kumar Lahiri
Nov 2, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Arijit Singha HazariGoutam Kumar Lahiri
Oct 30, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Sudip Kumar BeraGoutam Kumar Lahiri
Aug 14, 2020·Chemical Communications : Chem Comm·Sungho V ParkJohn F Berry
Aug 12, 2020·Chemistry, an Asian Journal·Sanchaita DeyGoutam Kumar Lahiri
Jan 19, 2021·Chemistry : a European Journal·Maya KumariGoutam Kumar Lahiri
Mar 9, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Madhumita ChatterjeeGoutam Kumar Lahiri
Jul 2, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Maya KumariGoutam Kumar Lahiri

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