Magnetocaloric Properties in Rare-Earth-Based Metal–Organic Frameworks: Influence of Magnetic Density and Hydrostatic Pressure

Vasile, Raluca Loredana; Silva, Romualdo S.; Céspedes, Eva; Martínez, José L.; Gutiérrez-Puebla, Enrique; Monge, M. Angeles; Gándara, Felipe

doi:10.1021/acs.inorgchem.3c03138

Cited by 2 publications

(1 citation statement)

References 43 publications

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“…This is due to Sm/Eu and Sr (nonmagnetic) elements sharing the same AA′-site in a 1:1 ratio, which leads to a large local magnetic disorder and unwanted loss of some Sm/Eu–O–Sm/Eu long-range ferromagnetic interactions, thereby significantly decreasing the Δ S M . Particularly, the smaller Δ S M compared to GdSrCoFeO 6 (∼13 J/kg K) is due to the peculiar feature of Gd in presenting a large spin ground state with zero orbital moment ( S = 7/2 and L = 0, i.e., J = 7/2) and the spherically symmetric ground state of 8 S 7/2 , which provides the largest entropy per single ion at low temperatures, unlike Sm and Eu. Furthermore, the strong lattice reorganization resulting from magnetoelastic coupling reinforces the magnetocaloric effect in GdSrCoFeO 6 at ∼8 K, which in the case of RSrCoFeO 6 (R = Sm, Eu) is also similarly observed around T N , but in a much smaller magnitude.…”

Section: Discussionmentioning

confidence: 99%

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO₆ (R = Sm, Eu) Double Perovskites

Silva,

Rodrigues,

Gainza

et al. 2024

Inorg. Chem.

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Double perovskite oxides, characterized by their tunable magnetic properties and robust interconnection between the lattice and magnetic degrees of freedom, present an enticing foundation for advanced magnetic refrigeration materials. Herein, we delve into the influence of rare-earth elements on RSrCoFeO 6 (R = Sm, Eu) disordered double perovskites by examining their structural, electronic, magnetic, and magnetocaloric properties. Temperature-dependent synchrotron X-ray diffraction analysis confirmed the stability of the orthorhombic phase (Pnma) across a wide temperature range. X-ray photoemission spectroscopy revealed that both Sm and Eu are in the 3+ state, whereas multiple states for Co 2+/3+ and Fe 3+/4+ are identified. The magnetic investigation and magnetocaloric effect (MCE) analysis brought to light the presence of a long-range antiferromagnetic (AFM) order with a second-order phase transition (SOPT) in both samples. The maximum magnetic entropy change ΔS M max was approximately 0.9 J/kg K for both samples at applied field 0−7 T, manifesting prominently above Neel temperatures T N ≈ 93 K (Sm) and 84 K (Eu). Nevertheless, different relative cooling powers (RCP) of 112.6 J/kg (Sm) and 95.5 J/kg (Eu) were observed. A detailed analysis of the temperature-dependent lattice parameters shed light on a distinct magnetocaloric effect across the magnetic transition temperature, unveiling an anisotropic thermal expansion [α V = 1.41 × 10 −5 K −1 (Sm) and α V = 1.54 × 10 −5 K −1 (Eu)] wherein the thermal expansion axial ratio α b Sm /α b Eu = 0.61 became lower with increasing temperature, which suggests that the Eu sample experiences a greater thermal expansion in the b-axis direction. At the atomic bonding level, the evidence for magnetoelastic coupling around the magnetic transition temperatures T N was found through the anomalies along the average Co/Fe−O bond distance, formal valence, octahedral distortion, as well as an anisotropic lattice expansion.

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Section: Discussionmentioning

confidence: 99%

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO₆ (R = Sm, Eu) Double Perovskites

Silva,

Rodrigues,

Gainza

et al. 2024

Inorg. Chem.

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Multifunctional self-refrigerated multivariate {GdLn} (Ln = Dy, Tb, Tb/Eu) metal–organic frameworks

Li,

Arauzo,

Roscini

et al. 2024

J. Mater. Chem. A

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Magnetocaloric Properties in Rare-Earth-Based Metal–Organic Frameworks: Influence of Magnetic Density and Hydrostatic Pressure

Cited by 2 publications

References 43 publications

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO₆ (R = Sm, Eu) Double Perovskites

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO₆ (R = Sm, Eu) Double Perovskites

Multifunctional self-refrigerated multivariate {GdLn} (Ln = Dy, Tb, Tb/Eu) metal–organic frameworks

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Magnetocaloric Properties in Rare-Earth-Based Metal–Organic Frameworks: Influence of Magnetic Density and Hydrostatic Pressure

Cited by 2 publications

References 43 publications

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO6 (R = Sm, Eu) Double Perovskites

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO6 (R = Sm, Eu) Double Perovskites

Multifunctional self-refrigerated multivariate {GdLn} (Ln = Dy, Tb, Tb/Eu) metal–organic frameworks

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Product

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Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO₆ (R = Sm, Eu) Double Perovskites

Magnetoelastic Coupling Evidence by Anisotropic Crossed Thermal Expansion in Magnetocaloric RSrCoFeO₆ (R = Sm, Eu) Double Perovskites