期刊
CHEMICAL SCIENCE
卷 9, 期 19, 页码 4477-4482出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8sc00961a
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences [DE-FG02-17ER16362]
- MRSEC program at the Materials Research Center [NSF DMR-1121262]
- International Institute for Nanotechnology (IIN)
- State of Illinois, through the IIN
Engendering electrical conductivity in high-porosity metal-organic frameworks (MOFs) promises to unlock the full potential of MOFs for electrical energy storage, electrocatalysis, or integration of MOFs with conventional electronic materials. Here we report that a porous zirconium-node-containing MOF, NU901, can be rendered electronically conductive by physically encapsulating C60, an excellent electron acceptor, within a fraction (ca. 60%) of the diamond-shaped cavities of the MOF. The cavities are defined by node-connected tetra-phenyl-carboxylated pyrene linkers, i. e. species that are excellent electron donors. The bulk electrical conductivity of the MOF is shown to increase from immeasurably low to 10 3 S cm 1, following fullerene incorporation. The observed conductivity originates from electron donor-acceptor interactions, i. e. charge-transfer interactions -a conclusion that is supported by density functional theory calculations and by the observation of a charge-transfer-derived band in the electronic absorption spectrum of the hybrid material. Notably, the conductive version of the MOF retains substantial nanoscale porosity and continues to display a sizable internal surface area, suggesting potential future applications that capitalize on the ability of the material to sorb molecular species.
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