Polyhedron p. 59 - 67 (2017)
Update date:2022-08-11
Topics:
Makhloufi, Gamall
Francis, Biju
Dechnik, Janina
Strzelczyk, Alexander
Janiak, Christoph
Fifteen microporous coordination polymers of symmetrical and flexible 4,4′-biphenyldiacetate (bpda2–) with lanthanide(III) cations (Ln3+) of formula {[Ln2(bpda)3(H2O)]?2H2O}n(Ln?=?La (1), Ce (2), Pr (3), Nd (4), Sm (5), Eu (6), Gd (7), Tb (8), Dy (9), Ho (10), Er (11), Tm (12), Yb (13), Lu (14), Y (15)), have been synthesized and characterized. Single crystal X-ray diffraction (for 1, 3 and 4) in combination with powder X-ray diffraction showed isostructural compounds with an infinite secondary building unit (SBU). In this SBU, two crystallographically independent lanthanide ions are connected by three carboxylate groups in chelating-bridging mode to zig-zag Ln-carboxylate chains. These chains are assembled by the biphenyl part of the ligand to a 3D network with water molecules in channels with rectangular cross-sections of ~1.6?×?3??2. Thermogravimetric analysis indicates complete removal of the water molecules at 150?°C and thermal stability up to 380?°C. Stability studies on compound 1 show no degeneration in crystallinity after refluxing in water or different organic solvents. The dehydrated compound 1 exhibited no N2or H2uptake at 77?K and no CH4or CO2uptake at 273?K up to 1?bar. High-pressure (17?bar, 273?K) CO2uptake of dehydrated [Ln2(bpda)3]ncorresponded to the formation of {[Ln2(bpda)3]·CO2}nwith about 40% of the adsorbed CO2retained upon desorption. Water vapor sorption of activated and hygroscopic [Ln2(bpda)3]nreformed {[Ln2(bpda)3(H2O)]·2H2O}n. 4,4′-Biphenyldiacetic acid (H2bpda) shows blue emission, its europium 6 and terbium 8 compounds show red and weak green luminescence under UV light irradiation, with the bpda2?ligand acting as an antenna ligand for the europium(III) ions.
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