Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 24, Pages 7411-7414Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b03604
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0018235]
- National Science Foundation [1122374]
- NSF [ACI-1053575]
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Partial oxidation of an iron-tetrazolate metal-organic framework (MOF) upon exposure to ambient atmosphere yields a mixed-valence material with single-crystal conductivities tunable over 5 orders of magnitude and exceeding 1 S/cm, the highest for a three-dimensionally connected MOF. Variable-temperature conductivity measurements reveal a small activation energy of 160 meV. Electronic spectroscopy indicates the population of midgap states upon air exposure and corroborates intervalence charge transfer between Fe3+ and Fe2+ centers. These findings are consistent with low-lying Fe3+ defect states predicted by electronic band structure calculations and demonstrate that inducing metal-based mixed valency is a powerful strategy toward realizing high and systematically tunable electrical conductivity in MOFs.
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