Mixed Yttrium and Dysprosium Lactates as First Example of Rare-Earth Hydrogen-Bonded Organic Framework Solid Solutions

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For the first time, molecular solid solutions of yttrium and dysprosium lactates of [Y1-xDyx(C3H5O3)3(H2O)2] composition, where x = 0, 0.01, 0.1, 0.5, 0.8, and 1, have been obtained. These can be considered the first solid solutions of rare-earth hydrogen-bonded organic framework (M-HOF). The obtained compounds were analyzed using a set of instrumental methods, including X-ray diffraction (XRD), Energy-dispersive X-ray spectroscopy (EDX), infrared (IR), and Raman spectroscopy. It has been shown that the unit cell volume of the lactate solid solutions linearly depends on their cationic composition. It has been established that changes in the cationic composition of the solid solutions result in a monotonic shift of the lines in the Raman spectra corresponding to Ln–O vibrations (151–158 cm–1). It has been demonstrated that the obtained compounds can be single-molecule magnets with an energy barrier of up to 108 K.

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M. Golikova

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences

Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991

A. Yapryntsev

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences

编辑信件的主要联系方式.
Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991

M. Teplonogova

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences; Lomonosov Moscow State University

Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991; Moscow, 119991

K. Babeshkin

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences

Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991

N. Efimov

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences

Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991

A. Baranchikov

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences

Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991

V. Ivanov

Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences; Lomonosov Moscow State University

Email: yapryntsev@igic.ras.ru
俄罗斯联邦, Moscow, 119991; Moscow, 119991

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3. Fig. 1. X-ray diffraction patterns of products obtained by hydrothermal treatment (70°C, 24 h) of a mixture of solutions of HMTA, L-lactic acid and yttrium/dysprosium chlorides in different ratios: a - in the absence of dysprosium chloride, b - Y : Dy = 99 : 1, c - Y : Dy = 90 : 10, d - Y : Dy = 50 : 50, e - Y : Dy = 20 : 80, f - in the absence of yttrium chloride.

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4. Fig. 2. Dependence on the cation composition of the unit cell volume of REE lactates [Y1-xDyx(C3H5O3)3(H2O)2] obtained by hydrothermal treatment (70°C, 24 h) of a mixture of solutions of HMTA, L-lactic acid and yttrium/dysprosium chlorides in different ratios.

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5. Fig. 3. Overview IR spectra of solid solutions of crystalline REE lactates of the composition [Y1-xDyx(C3H5O3)3(H2O)2] (a): x = 0, x = 0.01, x = 0.1, x = 0.5, x = 0.8, x = 1. Fragments of IR spectra of solid solutions of crystalline yttrium and dysprosium lactates in the ranges: 870-860 cm-1 (b) and 1130-1120 cm-1 (c). Denotations: ν - valence vibrations, as - asymmetric vibrations, s - symmetric vibrations, δ - strain vibrations, AL - vibrations of the hydroxyl group of lactate, r - pendulum vibrations, w - fan vibrations.

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6. Fig. 4. Overview CR spectra of solid solutions of crystalline REE lactates of the composition [Y1-xDyx(C3H5O3)3(H2O)2] (a): x = 0, x = 0.01, x = 0.1, x = 0.5, x = 0.8, x = 1. Fragment of the CR spectra of crystalline yttrium and dysprosium lactates in the range 140-170 cm-1 (b). Linear approximation of the position of the band maximum in the range 150-160 cm-1 (presumably the mode of Ln-O vibrations) (c). Denotations: ν - valence vibrations, as - asymmetric vibrations, s - symmetric vibrations, δ - strain vibrations, AL - vibrations of the hydroxyl group of lactate, r - pendulum vibrations, w - fan vibrations.

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7. Fig. 5. Temperature dependences of χT for compounds [Y1-xDyx(C3H5O3)3(H2O)2], where x = 1, 0.1, and 0.01 (H = 5000 E).

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8. Fig. 6. Dependence of relaxation times on the inverse temperature τ(1/T) in zero magnetic field for [Dy(C3H5O3)3(H2O)2] (a), [Y0.9Dy0.1(C3H5O3)3(H2O)2] (b) and [Y0.99Dy0.01(C3H5O3)3(H2O)2] (c). The blue line is the approximation of the high-temperature part by the Arrhenius equation. Red line - approximation by the sum of the Orbach and KTH relaxation processes.

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9. Fig. 7. Dependence of relaxation times on the inverse temperature τ(1/T) in a non-zero field for (a) [Dy(C3H5O3)3(H2O)2], (b) [Y0.9Dy0.1(C3H5O3)3(H2O)2], (c) [Y0.99Dy0.01(C3H5O3)3(H2O)2] The blue line is the approximation of the high-temperature part by the Arrhenius equation. Red line - approximation by the sum of (a) the Orbach and Raman processes, (b, c) the Orbach process and the direct relaxation process.

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