A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system

Rising global temperatures alongside increasing energy demand highlight the imperative for sustainable and energy-efficient refrigeration technologies. Magnetic refrigeration, based on the magnetocaloric effect (MCE), presents a compelling solid-state alternative to traditional vapor-compression sys...

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Authors: Guisado Arenas, Elisa, Cui, Zhe, Moreno Ramírez, Luis Miguel, Romero-Muñiz, Carlos, Law, Jia Yan, Franco García, Victorino
Format: article
Status:Published version
Publication Date:2026
Country:España
Institution:Universidad de Sevilla (US)
Repository:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:dnet:idus________::9f38160a11370f30770ce6e1d44087d3
Online Access:https://hdl.handle.net/11441/184137
https://doi.org/10.1088/2752-5724/ae36c5
Access Level:Open access
Keyword:Magnetocaloric effect
High entropy alloys
Low material criticality
Magnetostructural transformations
DFT calculations
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spelling A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi systemGuisado Arenas, ElisaCui, ZheMoreno Ramírez, Luis MiguelRomero-Muñiz, CarlosLaw, Jia YanFranco García, VictorinoMagnetocaloric effectHigh entropy alloysLow material criticalityMagnetostructural transformationsDFT calculationsRising global temperatures alongside increasing energy demand highlight the imperative for sustainable and energy-efficient refrigeration technologies. Magnetic refrigeration, based on the magnetocaloric effect (MCE), presents a compelling solid-state alternative to traditional vapor-compression systems. However, many high-performance magnetocaloric materials rely on critical elements such as rare earths, cobalt and germanium. Despite extensive compositional flexibility, high-entropy alloys (HEAs) have predominantly been investigated in equiatomic compositions incorporating significant quantities of highly critical elements to achieve large MCE or mixing rare-earth elements in majority proportions that only yield moderate MCE values, thereby failing to address issues of material criticality. In this study, we present a criticality-aware design strategy for the MnNiSi-HEA system, exemplifying a prototype of the latest third-generation HEAs. Various substitutional approaches were evaluated to achieve the coupling between magnetic and structural transitions. The most effective pathway, identified through the co-substitution of Fe and Cu reduces the structural transition temperature by over 900 K relative to MnNiSi while preserving the ferromagnetic characteristics of the low-temperature phase, successfully inducing a first-order magnetostructural transformation near room temperature. The resulting alloys, Mn0.5Fe0.5Ni1−xCuxSi, exhibit coupled transitionsspanning more than 100 K and demonstrate the highest MCE reported to date among HEAs free of cobalt, germanium and rare-earth elements, outperforming previous records by 360%. Complementary density functional theory calculations confirm the stability of the orthorhombic and hexagonal phases. Predictions of lattice entropy change closely match calorimetric measurements. This study establishes a new benchmark for low-criticality magnetocaloric HEAs, underscoring that optimal functional performance and sustainable material development can be achieved concomitantly. The proposed design methodology offers a valuable framework for advancing resource-resilient solid-state cooling materials and underscores the potential of HEAs as a platform for sustainable functional materials.IOP PublishingFísica de la Materia CondensadaAgencia Estatal de Investigación. EspañaMinisterio de Ciencia, Innovación y Universidades (MICIU). EspañaMinisterio de Hacienda y Función Pública2026info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfapplication/pdfhttps://hdl.handle.net/11441/184137https://doi.org/10.1088/2752-5724/ae36c5reponame:idUS. Depósito de Investigación de la Universidad de Sevillainstname:Universidad de Sevilla (US)InglésMaterials Future, 5 (2), 025601. PID2023-146047OB-I00PPIT2024-31833https://iopscience.iop.org/article/10.1088/2752-5724/ae36c5info:eu-repo/semantics/openAccessoai:dnet:idus________::9f38160a11370f30770ce6e1d44087d32026-06-17T12:51:07Z
dc.title.none.fl_str_mv A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
title A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
spellingShingle A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
Guisado Arenas, Elisa
Magnetocaloric effect
High entropy alloys
Low material criticality
Magnetostructural transformations
DFT calculations
title_short A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
title_full A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
title_fullStr A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
title_full_unstemmed A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
title_sort A criticality-aware design framework for sustainable magnetocaloric high-entropy alloys: the MnFeNiCuSi system
dc.creator.none.fl_str_mv Guisado Arenas, Elisa
Cui, Zhe
Moreno Ramírez, Luis Miguel
Romero-Muñiz, Carlos
Law, Jia Yan
Franco García, Victorino
author Guisado Arenas, Elisa
author_facet Guisado Arenas, Elisa
Cui, Zhe
Moreno Ramírez, Luis Miguel
Romero-Muñiz, Carlos
Law, Jia Yan
Franco García, Victorino
author_role author
author2 Cui, Zhe
Moreno Ramírez, Luis Miguel
Romero-Muñiz, Carlos
Law, Jia Yan
Franco García, Victorino
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv Física de la Materia Condensada
Agencia Estatal de Investigación. España
Ministerio de Ciencia, Innovación y Universidades (MICIU). España
Ministerio de Hacienda y Función Pública
dc.subject.none.fl_str_mv Magnetocaloric effect
High entropy alloys
Low material criticality
Magnetostructural transformations
DFT calculations
topic Magnetocaloric effect
High entropy alloys
Low material criticality
Magnetostructural transformations
DFT calculations
description Rising global temperatures alongside increasing energy demand highlight the imperative for sustainable and energy-efficient refrigeration technologies. Magnetic refrigeration, based on the magnetocaloric effect (MCE), presents a compelling solid-state alternative to traditional vapor-compression systems. However, many high-performance magnetocaloric materials rely on critical elements such as rare earths, cobalt and germanium. Despite extensive compositional flexibility, high-entropy alloys (HEAs) have predominantly been investigated in equiatomic compositions incorporating significant quantities of highly critical elements to achieve large MCE or mixing rare-earth elements in majority proportions that only yield moderate MCE values, thereby failing to address issues of material criticality. In this study, we present a criticality-aware design strategy for the MnNiSi-HEA system, exemplifying a prototype of the latest third-generation HEAs. Various substitutional approaches were evaluated to achieve the coupling between magnetic and structural transitions. The most effective pathway, identified through the co-substitution of Fe and Cu reduces the structural transition temperature by over 900 K relative to MnNiSi while preserving the ferromagnetic characteristics of the low-temperature phase, successfully inducing a first-order magnetostructural transformation near room temperature. The resulting alloys, Mn0.5Fe0.5Ni1−xCuxSi, exhibit coupled transitionsspanning more than 100 K and demonstrate the highest MCE reported to date among HEAs free of cobalt, germanium and rare-earth elements, outperforming previous records by 360%. Complementary density functional theory calculations confirm the stability of the orthorhombic and hexagonal phases. Predictions of lattice entropy change closely match calorimetric measurements. This study establishes a new benchmark for low-criticality magnetocaloric HEAs, underscoring that optimal functional performance and sustainable material development can be achieved concomitantly. The proposed design methodology offers a valuable framework for advancing resource-resilient solid-state cooling materials and underscores the potential of HEAs as a platform for sustainable functional materials.
publishDate 2026
dc.date.none.fl_str_mv 2026
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/11441/184137
https://doi.org/10.1088/2752-5724/ae36c5
url https://hdl.handle.net/11441/184137
https://doi.org/10.1088/2752-5724/ae36c5
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Materials Future, 5 (2), 025601.
PID2023-146047OB-I00
PPIT2024-31833
https://iopscience.iop.org/article/10.1088/2752-5724/ae36c5
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv IOP Publishing
publisher.none.fl_str_mv IOP Publishing
dc.source.none.fl_str_mv reponame:idUS. Depósito de Investigación de la Universidad de Sevilla
instname:Universidad de Sevilla (US)
instname_str Universidad de Sevilla (US)
reponame_str idUS. Depósito de Investigación de la Universidad de Sevilla
collection idUS. Depósito de Investigación de la Universidad de Sevilla
repository.name.fl_str_mv
repository.mail.fl_str_mv
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