期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 135, 期 36, 页码 13326-13329出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja407778a
关键词
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资金
- Center for Excitonics, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001088]
- NSF [CHE-9808061, DBI-9729592, CHE-0946721]
- Deutsche Forschungsgemeinschaft [RE3198/1-1]
We show that fluorescent molecules incorporated as ligands in rigid, porous metal-organic frameworks (MOFs) maintain their fluorescence response to a much higher temperature than in molecular crystals. The remarkable high-temperature ligand-based fluorescence, demonstrated here with tetraphenylethylene- and dihydroxyterephthalate-based linkers, is essential for enabling selective and rapid detection of analytes in the gas phase. Both Zn-2(TCPE) (TCPE = tetrakis(4-carboxyphenyl)ethylene) and Mg(H2DHBDC) (H2DHBDC2- = 2,5-dihydroxybenzene-1,4-dicarboxylate) function as selective sensors for ammonia at 100 degrees C, although neither shows NH3 selectivity at room temperature. Variable-temperature diffuse-reflectance infrared spectroscopy, fluorescence spectroscopy, and X-ray crystallography are coupled with density-functional calculations to interrogate the temperature-dependent guest-framework interactions and the preferential analyte binding in each material. These results describe a heretofore unrecognized, yet potentially general property of many rigid, fluorescent MOFs and portend new applications for these materials in selective sensors, with selectivity profiles that can be tuned as a function of temperature.
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