Control of Electronic Structure and Conductivity in Two-Dimensional Metal–Semiquinoid Frameworks of Titanium, Vanadium, and Chromium

Ziebel, Michael E.; Darago, Lucy E.; Long, Jeffrey R.

doi:10.1021/jacs.7b13510

Title: Control of Electronic Structure and Conductivity in Two-Dimensional Metal–Semiquinoid Frameworks of Titanium, Vanadium, and Chromium

Journal Article · Mon Feb 05 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b13510· OSTI ID:1460997

Ziebel, Michael E. ^[1]; Darago, Lucy E. ^[1];

^[2]

Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division

The isostructural, two-dimensional metal–organic frameworks (H₂NMe₂)₂M2(Cl₂dhbq)₃ (M = Ti, V; Cl₂dhbqn- = deprotonated 2,5-dichloro-3,6-dihydroxybenzoquinone) and (H₂NMe₂)_1.5Cr₂(dhbq)₃ (dhbq^n- = deprotonated 2,5-dihydroxybenzoquinone) are synthesized and investigated by spectroscopic, magnetic, and electrochemical methods. The three frameworks exhibit substantial differences in their electronic structures, and the bulk electronic conductivities of these phases correlate with the extent of delocalization observed via UV–vis–NIR and IR spectroscopies. Notably, substantial metal–ligand covalency in the vanadium phase results in the quenching of ligand-based spins, the observation of simultaneous metal- and ligand-based redox processes, and a high electronic conductivity of 0.45 S/cm. In conclusion, a molecular orbital analysis of these materials and a previously reported iron congener suggests that the differences in conductivity can be explained by correlating the metal–ligand energy alignment with the energy of intervalence charge transfer transitions, which should determine the barrier to charge hopping in the mixed-valence frameworks.

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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). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: SC0008688

OSTI ID:: 1460997

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 8; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Redox, transmetalation, and stacking properties of tetrathiafulvalene-2,3,6,7-tetrathiolate bridged tin, nickel, and palladium compounds Xie, Jiaze; Boyn, Jan-Niklas; Filatov, Alexander S. Chemical Science, Vol. 11, Issue 4 https://doi.org/10.1039/c9sc04381k	journal	January 2020
Coordination polymer-based conductive materials: ionic conductivity vs. electronic conductivity Wang, Hai-Ning; Meng, Xing; Dong, Long-Zhang Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/c9ta08253k	journal	January 2019
Recent Development and Application of Conductive MOFs Li, Pengfei; Wang, Bo Israel Journal of Chemistry, Vol. 58, Issue 9-10 https://doi.org/10.1002/ijch.201800078	journal	August 2018
Redox-active metal–organic frameworks for energy conversion and storage Calbo, Joaquín; Golomb, Matthias J.; Walsh, Aron Journal of Materials Chemistry A, Vol. 7, Issue 28 https://doi.org/10.1039/c9ta04680a	journal	January 2019
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
A new fluorone-based bridging ligand for discrete and polymeric assemblies including Mo and W based [4+4] metallocycles Sutton, Ashley L.; Abrahams, Brendan F.; Hudson, Timothy A. New Journal of Chemistry, Vol. 44, Issue 27 https://doi.org/10.1039/d0nj02413a	journal	January 2020