Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 133, Issue 12, Pages 4232-4235Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja111197d
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Funding
- NSF
- U.S. Department of Energy Office of Science (BES) [DE-SC0001011]
- Office of Energy Efficiency & Renewable Energy [DE-EE0003188]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [0906662] Funding Source: National Science Foundation
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0809776] Funding Source: National Science Foundation
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Diffusion-controlled luminescence quenching of a phosphorescent metal organic framework built from the Ru(bpy)(3)(2+)-derived bridging ligand (MOF-1) was studied using a series of amines of different sizes as quenchers. The dynamics of amine diffusion into solvent-filled MOF-1 channels was probed by modeling time-dependent luminescence quenching data, which provide quantitative diffusion coefficients for the amine quenchers. Triethylamine, tripropylamine, and tributylamine were found to follow Fickian diffusion with a diffusivity of (1.1 +/- 0.2) X 10(-13), (4.8 +/- 1.2) x 10(-14), and (4.0 +/- 0.4) x 10(-14) m(2)/s, respectively. Diisopropylethylamine (DIPEA), on the other hand, was found to be too large to enter the MOF channels. Despite its size, 4-MeOPhNPh2 can enter the MOF channels via a slow, complicated framework/guest intercalation process to result in extensive framework distortion as revealed by powder X-ray diffraction. This work represents the first quantitative study of the dynamics of molecular diffusion into solvent-filled MOF channels. Such quantitative information on molecular diffusion in MOFs is of fundamental importance to many of their potential applications (e.g., heterogeneous catalysis).
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