High Entropy: A General Strategy for Broadening the Operating Temperature of Magnetic Refrigeration

Feixiang Long; Yuzhu Song; Hengchao Li; Yuanji Xu; Fuyang Tian; Yuanpeng Zhang; Tianyu Li; Hui Liu; Jiazheng Hao; Lunhua He; Xianran Xing; Fengxia Hu; Jun Chen

doi:10.1021/jacs.4c14759

High Entropy: A General Strategy for Broadening the Operating Temperature of Magnetic Refrigeration

Feixiang Long, Yuzhu Song, Hengchao Li, Yuanji Xu, Fuyang Tian, Yuanpeng Zhang, Tianyu Li, Hui Liu, Jiazheng Hao, Lunhua He, Xianran Xing, Fengxia Hu, Jun Chen

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Abstract

Lattice distortion and disorder in the chemical environment of magnetic atoms within high-entropy compounds present intriguing issues in the modulation of magnetic functional compounds. However, the complexity inherent in high-entropy disordered systems has resulted in a relative scarcity of comprehensive investigations exploring the magnetic functional mechanisms of these alloys. Herein, we investigate the magnetocaloric effect (MCE) of the high-entropy intermetallic compound Gd_0.2Tb_0.2Dy_0.2Ho_0.2Er_0.2Co₂. Notably, the operating temperature range of the MCE broadens by an order of magnitude from 9 to 83 K while maintaining the refrigeration capacity compared to ErCo₂. Atomic-scale microstructure analysis and atomic pair distribution function measurements reveal that lattice distortion stabilizes the cubic structure and induces disorder in the chemical environment of magnetic atoms. First-principles calculations point out that the enhanced average correlation energy raises the Curie temperature. The random distribution of elements across these sites induces local magnetic disorder around magnetic atoms with lower correlation energy, broadening the operating temperature range of MCE. This study not only significantly advances the understanding of the magnetic behavior of high-entropy alloys but also promotes the research progress of high-entropy functional compounds.

Original language	English
Pages (from-to)	4349-4356
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	147
Issue number	5
DOIs	https://doi.org/10.1021/jacs.4c14759
State	Published - Feb 5 2025

Funding

This work was supported by the National Key R&D Program of China (2022YFE0109100), the Outstanding Young Scientist Program of Beijing Colleges and Universities (JWZQ20240101015), and the National Natural Science Foundation of China (22235002, 22275014, and 12104038). The use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The authors thank the Space Environment Simulation Research Infrastructure for help in our experiment. A portion of this work was performed on the Steady High Magnetic Field Facilities, High Magnetic Field Laboratory, CAS.

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title = "High Entropy: A General Strategy for Broadening the Operating Temperature of Magnetic Refrigeration",

abstract = "Lattice distortion and disorder in the chemical environment of magnetic atoms within high-entropy compounds present intriguing issues in the modulation of magnetic functional compounds. However, the complexity inherent in high-entropy disordered systems has resulted in a relative scarcity of comprehensive investigations exploring the magnetic functional mechanisms of these alloys. Herein, we investigate the magnetocaloric effect (MCE) of the high-entropy intermetallic compound Gd0.2Tb0.2Dy0.2Ho0.2Er0.2Co2. Notably, the operating temperature range of the MCE broadens by an order of magnitude from 9 to 83 K while maintaining the refrigeration capacity compared to ErCo2. Atomic-scale microstructure analysis and atomic pair distribution function measurements reveal that lattice distortion stabilizes the cubic structure and induces disorder in the chemical environment of magnetic atoms. First-principles calculations point out that the enhanced average correlation energy raises the Curie temperature. The random distribution of elements across these sites induces local magnetic disorder around magnetic atoms with lower correlation energy, broadening the operating temperature range of MCE. This study not only significantly advances the understanding of the magnetic behavior of high-entropy alloys but also promotes the research progress of high-entropy functional compounds.",

author = "Feixiang Long and Yuzhu Song and Hengchao Li and Yuanji Xu and Fuyang Tian and Yuanpeng Zhang and Tianyu Li and Hui Liu and Jiazheng Hao and Lunhua He and Xianran Xing and Fengxia Hu and Jun Chen",

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AU - Tian, Fuyang

AU - Zhang, Yuanpeng

AU - Li, Tianyu

AU - Liu, Hui

AU - Hao, Jiazheng

AU - He, Lunhua

AU - Xing, Xianran

AU - Hu, Fengxia

AU - Chen, Jun

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N2 - Lattice distortion and disorder in the chemical environment of magnetic atoms within high-entropy compounds present intriguing issues in the modulation of magnetic functional compounds. However, the complexity inherent in high-entropy disordered systems has resulted in a relative scarcity of comprehensive investigations exploring the magnetic functional mechanisms of these alloys. Herein, we investigate the magnetocaloric effect (MCE) of the high-entropy intermetallic compound Gd0.2Tb0.2Dy0.2Ho0.2Er0.2Co2. Notably, the operating temperature range of the MCE broadens by an order of magnitude from 9 to 83 K while maintaining the refrigeration capacity compared to ErCo2. Atomic-scale microstructure analysis and atomic pair distribution function measurements reveal that lattice distortion stabilizes the cubic structure and induces disorder in the chemical environment of magnetic atoms. First-principles calculations point out that the enhanced average correlation energy raises the Curie temperature. The random distribution of elements across these sites induces local magnetic disorder around magnetic atoms with lower correlation energy, broadening the operating temperature range of MCE. This study not only significantly advances the understanding of the magnetic behavior of high-entropy alloys but also promotes the research progress of high-entropy functional compounds.

AB - Lattice distortion and disorder in the chemical environment of magnetic atoms within high-entropy compounds present intriguing issues in the modulation of magnetic functional compounds. However, the complexity inherent in high-entropy disordered systems has resulted in a relative scarcity of comprehensive investigations exploring the magnetic functional mechanisms of these alloys. Herein, we investigate the magnetocaloric effect (MCE) of the high-entropy intermetallic compound Gd0.2Tb0.2Dy0.2Ho0.2Er0.2Co2. Notably, the operating temperature range of the MCE broadens by an order of magnitude from 9 to 83 K while maintaining the refrigeration capacity compared to ErCo2. Atomic-scale microstructure analysis and atomic pair distribution function measurements reveal that lattice distortion stabilizes the cubic structure and induces disorder in the chemical environment of magnetic atoms. First-principles calculations point out that the enhanced average correlation energy raises the Curie temperature. The random distribution of elements across these sites induces local magnetic disorder around magnetic atoms with lower correlation energy, broadening the operating temperature range of MCE. This study not only significantly advances the understanding of the magnetic behavior of high-entropy alloys but also promotes the research progress of high-entropy functional compounds.

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High Entropy: A General Strategy for Broadening the Operating Temperature of Magnetic Refrigeration

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