2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry

DeGayner, Jordan A.; Jeon, Ie -Rang; Sun, Lei; Dincă, Mircea; Harris, T. David

doi:10.1021/jacs.7b00705

Title: 2D Conductive Iron-Quinoid Magnets Ordering up to T_c = 105 K via Heterogenous Redox Chemistry

Journal Article · Thu Feb 23 00:00:00 EST 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b00705· OSTI ID:1388516

DeGayner, Jordan A. ^[1]; Jeon, Ie -Rang ^[1];

^[2];

^[1]

Northwestern Univ., Evanston, IL (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

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 (E_a = 0.26(1) cm^–1) and 1.0(3) × 10^–3 S/cm (E_a = 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 [Fe^III₂(L^3–•)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 T_c = 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 E_a = 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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)

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

Grant/Contract Number:: SC0001088; AC02-06CH11357; NNCI-154220; ECCS-154220; DMR-112126; DMR-135195

OSTI ID:: 1388516

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 11; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 168 works

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Title: 2D Conductive Iron-Quinoid Magnets Ordering up to Tc = 105 K via Heterogenous Redox Chemistry

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Title: 2D Conductive Iron-Quinoid Magnets Ordering up to T_c = 105 K via Heterogenous Redox Chemistry