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Terbium and Europium Chlorocyananilate-Based 2D Coordination Polymers
Mariangela Oggianu1,2, Alexandre Abhervé3, Daniela Marongiu4
1Department of Chemical and Geological Sciences, University of Cagliari, Highway 554, Crossroads for Sestu, I-09042 Monserrato, Italy.
Molecules (Basel, Switzerland)
|September 28, 2023
Summary
New two-dimensional layered coordination polymers using lanthanide ions (Tb and Eu) and a novel benzoquinone ligand were synthesized. These materials exhibit distinct structural properties and potential for exfoliation into ultrathin nanosheets.
Area of Science:
- Materials Science
- Inorganic Chemistry
- Crystallography
Background:
- Two-dimensional (2D) coordination polymers offer unique properties due to their layered structures.
- Lanthanide ions (LnIII) are crucial for developing functional materials with specific magnetic and optical properties.
- Benzoquinone derivatives serve as versatile ligands in coordination chemistry.
Purpose of the Study:
- To synthesize and characterize novel 2D layered coordination polymers incorporating lanthanide ions (terbium and europium) and a hetero-substituted 3-chloro-6-cyano-2,5-dihydroxybenzoquinone ligand (ClCNAn2-).
- To investigate the structural differences between the synthesized terbium (Tb) and europium (Eu) compounds and their intermediates.
- To explore the exfoliation potential of the resulting 2D materials and their magnetic properties.
Main Methods:
- Conventional one-pot synthesis for polyhydrated intermediates and recrystallization from DMSO for the final compounds.
- X-ray powder diffraction (XRPD) for phase identification and structural analysis.
- Liquid-assisted sonication for exfoliation of 2D nanosheets and atomic force microscopy (AFM) for characterization.
Main Results:
- Two series of LnIII coordination polymers, Ln2(ClCNAn)3(DMSO)6 (1 and 2) and Ln2(ClCNAn)3(H2O)x·yH2O (1' and 2'), were successfully synthesized.
- Compounds 1 (Tb) and 2 (Eu) are not isostructural, with compound 1 featuring a 2D coordination framework of 3,6 topology forming distorted hexagons, while compound 2 exhibits flat, non-corrugated 2D sheets.
- Ultrathin nanosheets of compound 1 were obtained via exfoliation, confirming its 2D nature. Magnetic studies on compound 1 suggest crystal-field level depopulation.
Conclusions:
- The study reports the successful synthesis of novel TbIII and EuIII coordination polymers with a unique benzoquinone ligand, yielding distinct 2D layered structures.
- The ability to exfoliate these materials into ultrathin nanosheets opens avenues for their application in advanced material science.
- Structural variations between the Tb and Eu analogues highlight the subtle influence of lanthanide ions on framework assembly and properties.
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