2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry
Abstract
We report the magnetism and conductivity for a redox pair of iron-quinoid metal–organic frameworks (MOFs). The oxidized compound, (Me2NH2)2[Fe2L3]·2H2O·6DMF (LH2 = 2,5-dichloro-3,6-dihydroxo-1,4-benzoquinone) was previously shown to magnetically order below 80 K in its solvated form, with the ordering temperature decreasing to 26 K upon desolvation. Here, we demonstrate this compound to exhibit electrical conductivity values up to σ = 1.4(7) × 10–2 S/cm (Ea = 0.26(1) cm–1) and 1.0(3) × 10–3 S/cm (Ea = 0.19(1) cm–1) in its solvated and desolvated forms, respectively. Upon soaking in a DMF solution of Cp2Co, the compound undergoes a single-crystal-to-single-crystal one-electron reduction to give (Cp2Co)1.43(Me2NH2)1.57[Fe2L3]·4.9DMF. Structural and spectroscopic analysis confirms this reduction to be ligand-based, and as such the trianionic framework is formulated as [FeIII2(L3–•)3]3–. Magnetic measurements for this reduced compound reveal the presence of dominant intralayer metal–organic radical coupling to give a magnetically ordered phase below Tc = 105 K, one of the highest reported ordering temperatures for a MOF. This high ordering temperature is significantly increased relative to the oxidized compound, and stems from the overall increase in coupling strength afforded by an additional organic radical. In line with the high critical temperature, the new MOF exhibits magnetic hysteresis up to 100more »
- Authors:
-
[2];
[2];
[1]
- Northwestern Univ., Evanston, IL (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1388516
- Grant/Contract Number:
- SC0001088; AC02-06CH11357; NNCI-154220; ECCS-154220; DMR-112126; DMR-135195
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 11; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); solid state lighting; photosynthesis (natural and artificial); charge transport; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)
Citation Formats
DeGayner, Jordan A., Jeon, Ie -Rang, Sun, Lei, Dincă, Mircea, and Harris, T. David. 2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry. United States: N. p., 2017.
Web. doi:10.1021/jacs.7b00705.
DeGayner, Jordan A., Jeon, Ie -Rang, Sun, Lei, Dincă, Mircea, & Harris, T. David. 2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry. United States. https://doi.org/10.1021/jacs.7b00705
DeGayner, Jordan A., Jeon, Ie -Rang, Sun, Lei, Dincă, Mircea, and Harris, T. David. Thu .
"2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry". United States. https://doi.org/10.1021/jacs.7b00705. https://www.osti.gov/servlets/purl/1388516.
@article{osti_1388516,
title = {2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry},
author = {DeGayner, Jordan A. and Jeon, Ie -Rang and Sun, Lei and Dincă, Mircea and Harris, T. David},
abstractNote = {We report the magnetism and conductivity for a redox pair of iron-quinoid metal–organic frameworks (MOFs). The oxidized compound, (Me2NH2)2[Fe2L3]·2H2O·6DMF (LH2 = 2,5-dichloro-3,6-dihydroxo-1,4-benzoquinone) was previously shown to magnetically order below 80 K in its solvated form, with the ordering temperature decreasing to 26 K upon desolvation. Here, we demonstrate this compound to exhibit electrical conductivity values up to σ = 1.4(7) × 10–2 S/cm (Ea = 0.26(1) cm–1) and 1.0(3) × 10–3 S/cm (Ea = 0.19(1) cm–1) in its solvated and desolvated forms, respectively. Upon soaking in a DMF solution of Cp2Co, the compound undergoes a single-crystal-to-single-crystal one-electron reduction to give (Cp2Co)1.43(Me2NH2)1.57[Fe2L3]·4.9DMF. Structural and spectroscopic analysis confirms this reduction to be ligand-based, and as such the trianionic framework is formulated as [FeIII2(L3–•)3]3–. Magnetic measurements for this reduced compound reveal the presence of dominant intralayer metal–organic radical coupling to give a magnetically ordered phase below Tc = 105 K, one of the highest reported ordering temperatures for a MOF. This high ordering temperature is significantly increased relative to the oxidized compound, and stems from the overall increase in coupling strength afforded by an additional organic radical. In line with the high critical temperature, the new MOF exhibits magnetic hysteresis up to 100 K, as revealed by variable-field measurements. Lastly, this compound is electrically conductive, with values up to σ = 5.1(3) × 10–4 S/cm with Ea = 0.34(1) eV. Taken together, these results demonstrate the unique ability of metal-quinoid MOFs to simultaneously exhibit both high magnetic ordering temperatures and high electrical conductivity.},
doi = {10.1021/jacs.7b00705},
journal = {Journal of the American Chemical Society},
number = 11,
volume = 139,
place = {United States},
year = {Thu Feb 23 00:00:00 EST 2017},
month = {Thu Feb 23 00:00:00 EST 2017}
}
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