期刊
JOURNAL OF MATERIALS CHEMISTRY
卷 22, 期 39, 页码 21210-21217出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2jm34088g
关键词
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资金
- National Basic Research Program of China (973 Program) [2012CB821702]
- National Natural Science Foundation of China [21173221, 21233009]
- State Key Laboratory of Structural Chemistry and Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
New luminescent lanthanide-carboxylate frameworks, formulated as [Ln(4)(m-BDC)(6)(H2O)(4)(DMF)]center dot(H2O)(2)center dot(DMF) (Ln = Eu 1; Gd 2; Tb 3) (m-H2BDC 1,3-benzenedicarboxylic acid) have been solvo(hydro) thermally synthesized. Single-crystal X-ray diffraction studies reveal that compounds 1-3 are isomorphous and each displays a layered structure constructed by helical lanthanide-carboxylate chains. DFT and TD-DFT calculations were conducted in detail to discuss the energy levels, including the HOMO, LUMO, singlet and triplet energies of the m-H2BDC ligand. The results indicate that the m-BDC2- dianion acts as an antenna chromophore that is able to efficiently absorb and transfer energy to the lanthanide ions. Compounds 1-3 all exhibit high thermostability and are stable up to 450 degrees C, as confirmed by the TGA and temperature-dependent PXRD experiments. Compounds 1 and 3 are strong luminescent materials. Compound 3 is among some of the best examples of luminescent lanthanide compounds, with highly efficient emission quantum yields of 81.40% at 77 K, 75.37% at room temperature and 56.64% after calcination at 450 degrees C, respectively. In addition, the energy transfer processes for compounds 1 and 3 have also been studied and illustrated in detail.
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