期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 1, 期 47, 页码 14982-14989出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3ta14009a
关键词
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资金
- UNC EFRC: Center for Solar Fuels, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- NSF [DMR-0906662]
- DOE [DE-FG02-06ER15788]
Two non-porous metal-organic frameworks (MOFs) with caged Ru(bpy)(3)(2+) chromophores, [Ru(bpy)(3)][-Zn-2(C2O4)(3)] (1) and [Ru(bpy)(3)][NaAl(C2O4)(3)] (2), were synthesized and characterized. Their emission properties were studied by both steady-state and time-resolved luminescence measurements. Air-free microcrystals of 1 and 2 exhibit long-lived triplet metal-to-ligand charge transfer ((MLCT)-M-3) excited states with lifetimes of 760 and 1305 ns, respectively. Lifetimes are significantly shortened (to 92 ns for 1 and 144 ns for 2) by trapping of trace amounts of oxygen in the non-porous MOFs, presumably due to amplified luminescence quenching of Ru(bpy)(3)(2+)*. Following MLCT excitation, Ru(bpy)(3)(2+)*/Ru(bpy)(3)(2+) energy transfer migration in 1 and 2 results in efficient quenching of Ru(bpy)(3)(2+)* by Os(bpy)(3)(2+) added as an energy transfer trap at doping levels of 0.2-1.0%. A kinetic analysis indicates that the three-dimensional chromophore connectivity in 1 and 2 provides a network for rapid excited state energy transfer migration among Ru(bpy)(3)(2+) units, ultimately, finding an Os(bpy)(3)(2+) trap site. These crystalline frameworks with caged chromophores have proven to be ideal systems for studying light harvesting processes in artificial supramolecular systems.
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