Electronic Conductivity, Ferrimagnetic Ordering, and Reductive Insertion Mediated by Organic Mixed-Valence in a Ferric Semiquinoid Metal–Organic Framework

Darago, Lucy E.; Aubrey, Michael L.; Yu, Chung Jui; Gonzalez, Miguel I.; Long, Jeffrey R.

doi:10.1021/jacs.5b10385

Title: Electronic Conductivity, Ferrimagnetic Ordering, and Reductive Insertion Mediated by Organic Mixed-Valence in a Ferric Semiquinoid Metal–Organic Framework

Journal Article · Tue Nov 17 00:00:00 EST 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b10385· OSTI ID:1488852

Darago, Lucy E. ^[1]; Aubrey, Michael L. ^[1]; Yu, Chung Jui ^[1]; Gonzalez, Miguel I. ^[1]; Long, Jeffrey R. ^[2]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Here, a three-dimensional network solid composed of Fe^III centers and paramagnetic semiquinoid linkers, (NBu₄)₂Fe^III₂(dhbq₎₃ (dhbq2–/3– = 2,5-dioxidobenzoquinone/1,2-dioxido-4,5-semiquinone), is shown to exhibit a conductivity of 0.16 ± 0.01 S/cm at 298 K, one of the highest values yet observed for a metal–organic framework (MOF). The origin of this electronic conductivity is determined to be ligand mixed-valency, which is characterized using a suite of spectroscopic techniques, slow-scan cyclic voltammetry, and variable-temperature conductivity and magnetic susceptibility measurements. Importantly, UV–vis–NIR diffuse reflectance measurements reveal the first observation of Robin–Day Class II/III mixed valency in a MOF. Pursuit of stoichiometric control over the ligand redox states resulted in synthesis of the reduced framework material Na_0.9(NBu₄)_1.8Fe^III₂(dhbq)₃. Differences in electronic conductivity and magnetic ordering temperature between the two compounds are investigated and correlated to the relative ratio of the two different ligand redox states. Overall, the transition metal–semiquinoid system is established as a particularly promising scaffold for achieving tunable long-range electronic communication in MOFs.

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Research Organization:: Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Beamline 17-BM; Beamline 11.3.1

Grant/Contract Number:: FG02-12ER16362; SC0008688

OSTI ID:: 1488852

Journal Information:: Journal of the American Chemical Society, Vol. 137, Issue 50; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 273 works

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An Organic Mixed-Valence Ligand for Multistate Redox-Active Coordination Networks Ha, Joo Yeon; Koo, Jin Young; Ohtsu, Hiroyoshi Angewandte Chemie, Vol. 130, Issue 17 https://doi.org/10.1002/ange.201713035	journal	March 2018
Titelbild: A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity (Angew. Chem. 13/2020) Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan Angewandte Chemie, Vol. 132, Issue 13 https://doi.org/10.1002/ange.202001277	journal	January 2020
Cover Picture: A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity (Angew. Chem. Int. Ed. 13/2020) Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan Angewandte Chemie International Edition, Vol. 59, Issue 13 https://doi.org/10.1002/anie.202001277	journal	March 2020
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