Magnetocaloric Ln(HCO2)(C2O4) frameworks: synthesis, structure and magnetic properties

Mario Falsaperna; Gavin B.G. Stenning; Ivan da Silva; Paul J. Saines

doi:10.1039/d1tc01831k

Magnetocaloric Ln(HCO₂)(C₂O₄) frameworks: synthesis, structure and magnetic properties

Mario Falsaperna, Gavin B.G. Stenning, Ivan da Silva, Paul J. Saines

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

8 Citations (SciVal)

Abstract

This study probes the structure and the magnetic properties of members of the Ln(HCO₂)(C₂O₄) (Ln = Sm³⁺-Er³⁺) family of coordination frameworks. These frameworks adoptPnmaorthorhombic symmetry with one-dimensional chains arranged on a distorted triangular lattice. The magnetic properties of the Gd-Ho members of this series indicate they remain paramagnetic down to 2 K, with Dy(HCO₂)(C₂O₄) magnetically ordering at 0.6 K. The magnetocaloric effect of Gd(HCO₂)(C₂O₄) is amongst the highest found in frameworks with a peak entropy change of 55.97 J kg⁻¹K⁻¹(218.42 mJ cm⁻³K⁻¹) for a 5-0 T field change atT_max= 2 K, making this material a very good candidate for ultra-low temperature magnetic cooling. In contrast with related magnetocaloric materials lanthanides with high magnetocrystalline anisotropy do not generally improve the magnetocaloric performance of this family at higher temperatures and lower fields. Neutron diffraction experiments suggest that Tb(HCO₂)(C₂O₄) and Ho(HCO₂)(C₂O₄) lack significant local magnetic correlations, highlighting the key role these play in optimising the magnetocaloric performance in low fields in related phases; this emphasises the importance of designing materials with specific magnetic interactions to optimise magnetocaloric performance.

Original language	English
Pages (from-to)	13209-13217
Number of pages	9
Journal	Journal of Materials Chemistry C
Volume	9
Issue number	38
Early online date	26 Aug 2021
DOIs	https://doi.org/10.1039/d1tc01831k
Publication status	Published - 14 Oct 2021

Bibliographical note

Publisher Copyright:
© The Royal Society of Chemistry 2021.

Funding

We would like to thank the Leverhulme Trust and Engineering and Physical Sciences Research Council for funding this work through RPG-2018-268 and EP/T027886/1, respectively. We would also like to thank the Science and Technologies Facilities Council for granting experiment time on the GEM powder diffractometer at the ISIS Neutron and Muon Source.

Funders	Funder number
ISIS Neutron and Muon Source
Engineering and Physical Sciences Research Council	EP/T027886/1, RPG-2018-268
Science and Technology Facilities Council
Leverhulme Trust

ASJC Scopus subject areas

General Chemistry
Materials Chemistry

Access to Document

10.1039/d1tc01831kLicence: CC BY

Cite this

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title = "Magnetocaloric Ln(HCO2)(C2O4) frameworks: synthesis, structure and magnetic properties",

abstract = "This study probes the structure and the magnetic properties of members of the Ln(HCO2)(C2O4) (Ln = Sm3+-Er3+) family of coordination frameworks. These frameworks adoptPnmaorthorhombic symmetry with one-dimensional chains arranged on a distorted triangular lattice. The magnetic properties of the Gd-Ho members of this series indicate they remain paramagnetic down to 2 K, with Dy(HCO2)(C2O4) magnetically ordering at 0.6 K. The magnetocaloric effect of Gd(HCO2)(C2O4) is amongst the highest found in frameworks with a peak entropy change of 55.97 J kg−1K−1(218.42 mJ cm−3K−1) for a 5-0 T field change atTmax= 2 K, making this material a very good candidate for ultra-low temperature magnetic cooling. In contrast with related magnetocaloric materials lanthanides with high magnetocrystalline anisotropy do not generally improve the magnetocaloric performance of this family at higher temperatures and lower fields. Neutron diffraction experiments suggest that Tb(HCO2)(C2O4) and Ho(HCO2)(C2O4) lack significant local magnetic correlations, highlighting the key role these play in optimising the magnetocaloric performance in low fields in related phases; this emphasises the importance of designing materials with specific magnetic interactions to optimise magnetocaloric performance.",

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