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 UTC 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. ^[2]; Yu, Chung Jui ^[2]; Gonzalez, Miguel I. ^[2]; Long, Jeffrey R. ^[3]

Univ. of California, Berkeley, CA (United States); Nanoporous Materials Genome Center
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) (SC-22)

Contributing Organization:: Beamline 11.3.1; Beamline 17-BM

Grant/Contract Number:: SC0008688

OSTI ID:: 1488852

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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A Dual‐Ligand Porous Coordination Polymer Chemiresistor with Modulated Conductivity and Porosity Yao, Ming‐Shui; Zheng, Jia‐Jia; Wu, Ai‐Qian Angewandte Chemie, Vol. 132, Issue 1 https://doi.org/10.1002/ange.201909096	journal	November 2019
On‐surface Synthesis of a Semiconducting 2D Metal–Organic Framework Cu ₃ (C ₆ O ₆ ) Exhibiting Dispersive Electronic Bands Zhang, Ran; Liu, Jing; Gao, Yifan Angewandte Chemie, Vol. 132, Issue 7 https://doi.org/10.1002/ange.201913698	journal	January 2020
A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan Angewandte Chemie, Vol. 132, Issue 13 https://doi.org/10.1002/ange.201914395	journal	January 2020
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
Layer-by-Layer Assembled Conductive Metal-Organic Framework Nanofilms for Room-Temperature Chemiresistive Sensing Yao, Ming-Shui; Lv, Xiao-Jing; Fu, Zhi-Hua Angewandte Chemie International Edition, Vol. 56, Issue 52 https://doi.org/10.1002/anie.201709558	journal	November 2017
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Thermally Induced Valence Tautomeric Transition in a Two-Dimensional Fe-Tetraoxolene Honeycomb Network Chen, Jian; Sekine, Yoshihiro; Komatsumaru, Yuki Angewandte Chemie International Edition, Vol. 57, Issue 37 https://doi.org/10.1002/anie.201807556	journal	August 2018
A Dual‐Ligand Porous Coordination Polymer Chemiresistor with Modulated Conductivity and Porosity Yao, Ming‐Shui; Zheng, Jia‐Jia; Wu, Ai‐Qian Angewandte Chemie International Edition, Vol. 59, Issue 1 https://doi.org/10.1002/anie.201909096	journal	January 2020
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A Series of Early Lanthanide Chloranilate Frameworks with a Square Grid Topology Hua, Carol; Tay, Hui Min; He, Qilin Australian Journal of Chemistry, Vol. 72, Issue 10 https://doi.org/10.1071/ch19193	journal	January 2019
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Designing Kitaev Spin Liquids in Metal-Organic Frameworks Yamada, Masahiko G.; Fujita, Hiroyuki; Oshikawa, Masaki Physical Review Letters, Vol. 119, Issue 5 https://doi.org/10.1103/physrevlett.119.057202	journal	August 2017
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