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Synthesis, crystal structures and magnetic properties of two heterometallic {Ln₈Cr₄} (Ln = Gd³⁺ and Tb³⁺) complexes with one-dimensional wave chain structure.

ABSTRACT: Two isomorphic heterometallic 3d-4f cluster-based materials, formulated [Gd₈Cr₄(IN)₁₈(μ₃-O)₂(μ₃-OH)₆(μ₄-O)₄(H₂O)₁₀]·13H₂O (1) and [Tb₈Cr₄(IN)₁₈(μ₃-O)₂(μ₃-OH)₆(μ₄-O)₄(H₂O)₁₀]·13H₂O (2) (abbreviation: {Ln₈Cr₄}: Ln = Gd³⁺ (1); Tb³⁺ (2); HIN = isonicotinic acid), were achieved by hydro-/solvothermal method through using the ligand HIN. X-ray diffraction analysis illustrates eight lanthanide ions (Ln = Gd³⁺, Tb³⁺) and four transition-metal ions (Cr³⁺) of {Ln₈Cr₄} were constructed from two classical "drum-like" {Ln₄Cr₂} structures associated by organic ligands HIN, displaying a one-dimensional wave chain structure, which is rare. The magnetic properties of {Gd₈Cr₄} were inspected and showed the existence of antiferromagnetic coupling interactions between contiguous metal ions. On top of this, the magnetic entropy change of ΔS _m can attain 23.40 J kg^-1 K^-1 (44.90 mJ cm^-3 K^-1) at about 3 K and ΔH = 7 T. Besides, fluorescence measurements of {Tb₈Cr₄} display typical characteristic Tb-based luminescence.

SUBMITTER: Han YM

PROVIDER: S-EPMC9050496 | biostudies-literature | 2020 Mar

REPOSITORIES: biostudies-literature

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Synthesis, crystal structures and magnetic properties of two heterometallic {Ln8Cr4} (Ln = Gd3+ and Tb3+) complexes with one-dimensional wave chain structure.

Han Ye-Min YM Li Ning-Fang NF Yu Yan-Zhao YZ Cao Jia-Peng JP Yang Mu-Xiu MX Hong Ya-Lin YL Kang Run-Kun RK Yuan Peng P Xu Yan Y

RSC advances 20200320 19

Two isomorphic heterometallic 3d-4f cluster-based materials, formulated [Gd8Cr4(IN)18(μ3-O)2(μ3-OH)6(μ4-O)4(H2O)10]·13H2O (1) and [Tb8Cr4(IN)18(μ3-O)2(μ3-OH)6(μ4-O)4(H2O)10]·13H2O (2) (abbreviation: {Ln8Cr4}: Ln = ...[more]

PMID: 35495346

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Project description:We have investigated the incorporation of the luminescent Eu3+ cation in different LnPO4 (Ln = Tb, Gd1-xLu x , x = 0.3, 0.5, 0.7, 1) host phases. All samples were analyzed with powder X-ray diffraction (PXRD), Raman spectroscopy, and site-selective time-resolved laser-induced luminescence spectroscopy (TRLFS) directly after synthesis and after an aging time of one year at ambient conditions. The PXRD investigations demonstrate the formation of a TbPO4 phase in an uncommon anhydrite-like crystal structure evoked by a pressure-induced preparation step (grinding). In the Gd1-xLu x PO4 solid solution series, several different crystal structures are observed depending on the composition. The TRLFS emission spectra of LuPO4, Gd0.3Lu0.7PO4, and Gd0.5Lu0.5PO4 indicate Eu3+-incorporation within a xenotime-type crystal structure. TRLFS and PXRD investigations of the Gd0.7Lu0.3PO4 composition show the presence of anhydrite, xenotime, and monazite phases, implying that xenotime no longer is the favored crystal structure due to the predominance of the substantially larger Gd3+-cation in this solid phase. Eu3+-incorporation occurs predominantly in the anhydrite-like structure with smaller contributions of Eu3+ incorporated in monazite and xenotime. The electronic levels of the Eu3+-dopant in Gd0.3Lu0.7PO4 and Gd0.5Lu0.5PO4 xenotime hosts are strongly coupled to external lattice vibrations, giving rise to high-energy peaks in the obtained excitation spectra. The coupling becomes stronger after aging to such an extent that direct excitation of Eu3+ in the xenotime structure is strongly suppressed. This phenomenon, however, is only visible for materials where Eu3+ was predominantly incorporated within the xenotime structure. Single crystals of Eu3+-doped LuPO4 show no changes upon aging despite the presence of vibronically coupled excitation peaks in the excitation spectra measured directly after synthesis. Based on this observation, we propose a lattice relaxation process occurring in the powder samples during aging, resulting in Eu3+ migration within the crystal structure and Eu3+ accumulation at grain boundaries or xenotime surface sites.

Dataset Information

Synthesis, crystal structures and magnetic properties of two heterometallic {Ln₈Cr₄} (Ln = Gd³⁺ and Tb³⁺) complexes with one-dimensional wave chain structure.

Publications

Synthesis, crystal structures and magnetic properties of two heterometallic {Ln<sub>8</sub>Cr<sub>4</sub>} (Ln = Gd<sup>3+</sup> and Tb<sup>3+</sup>) complexes with one-dimensional wave chain structure.

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