Highly luminescent and thermostable lanthanide-carboxylate framework materials with helical configurations

Huabin Zhang, Liujiang Zhou, Jing Wei, Zhihua Li, Ping Lin, Shaowu Du

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108 Scopus citations

Abstract

New luminescent lanthanide-carboxylate frameworks, formulated as [Ln 4(m-BDC)6(H2O)4(DMF)]·(H 2O)2·(DMF) (Ln = Eu 1; Gd 2; Tb 3) (m-H 2BDC = 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 °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 °C, respectively. In addition, the energy transfer processes for compounds 1 and 3 have also been studied and illustrated in detail. © 2012 The Royal Society of Chemistry.
Original languageEnglish (US)
Pages (from-to)21210-21217
Number of pages8
JournalJournal of Materials Chemistry
Volume22
Issue number39
DOIs
StatePublished - Oct 21 2012
Externally publishedYes

ASJC Scopus subject areas

  • Materials Chemistry
  • General Chemistry

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