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Iron(II) Complexes Featuring a Redox-Active Dihydrazonopyrrole Ligand

preprint
submitted on 18.03.2021, 16:05 and posted on 19.03.2021, 12:37 by Kate Jesse, Mu-Chieh Chang, Alexander S. Filatov, John Anderson
Nature uses control of the secondary coordination sphere
to facilitate an astounding variety of transformations. Similarly, synthetic chemists have found metal-ligand cooperativity to be a powerful strategy for designing complexes that can mediate challenging reactivity. In particular, this strategy has been used to facilitate two electron reactions with first row transition metals that
more typically engage in one electron redox processes. While NNN pincer ligands feature prominently in this area, examples which can potentially engage in both proton and electron transfer are less common. Dihydrazonopyrrole (DHP) ligands have been isolated in a variety of redox and protonation states when complexed to Ni. However, the redox-state of this ligand scaffold is less obvious when
complexed to metal centers with more accessible redox couples. Here, we synthesize a new series of Fe-DHP complexes in two distinct oxidation states. Detailed characterization supports that the redox chemistry
in this set is still primarily ligand based. Finally, these
complexes exist as 5-coordinate species with an open coordination site offering the possibility of enhanced reactivity.

Funding

R35 GM133470

FG-2019-11497

NSF/CHE-1834750

DE-AC02-06CH11357

History

Email Address of Submitting Author

jsanderson@uchicago.edu

Institution

University of Chicago

Country

United States of America

ORCID For Submitting Author

0000-0002-0730-3018

Declaration of Conflict of Interest

None

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