Using high pressure to investigate the stability of a high entropy wurtzite structured (MnFeCuAgZnCd)S

Mark A. Buckingham; Joshua J. Shea; Kho Zhi Quan; Pok Man Ethan Lo; Joshua Swindell; Weichen Xiao; David J. Lewis; Alex S. Eggeman; Simon A. Hunt

doi:10.1038/s42004-025-01463-9

Using high pressure to investigate the stability of a high entropy wurtzite structured (MnFeCuAgZnCd)S

Mark A. Buckingham, Joshua J. Shea, Kho Zhi Quan, Pok Man Ethan Lo, Joshua Swindell, Weichen Xiao, David J. Lewis, Alex S. Eggeman, Simon A. Hunt

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

Abstract

High entropy metal chalcogenides are an emergent class of materials that have shown exceptional promise in applications such as energy storage, catalysis, and thermoelectric energy conversion. However, the stability of these materials to factors other than temperature are as yet unknown. Here we set out to assess the stability of the high entropy metal sulfide (MnFeCuAgZnCd)S with high pressure (up to 9 GPa), compared to an enthalpically stabilised Ag₃CuS₂, and a quasi-stable (MnFeZnCd)S. Compression and pressure-annealing of (MnFeCuAgZnCd)S showed diffusion-controlled time and pressure dependent exsolution of jalpaite (Ag₃CuS₂) from the bulk. Bulk materials characterisation found minor phase impurities and possible elemental localisations in (MnFeCuAgZnCd)S prior to pressure-annealing. To gain deeper understanding of the material pre- and post-pressure annealing at the nanoscale an advanced technique was used which combined machine learning, unsupervised clustering analysis of STEM-EDX mapping with scanning precession electron diffraction (SPED), which revealed a chemically distinct post-pressure annealed jalpaite exsolved from (MnFeCuAgZnCd)S.

Original language	English
Article number	65
Journal	Communications Chemistry
Volume	8
Issue number	1
DOIs	https://doi.org/10.1038/s42004-025-01463-9
Publication status	Published - 5 Mar 2025

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title = "Using high pressure to investigate the stability of a high entropy wurtzite structured (MnFeCuAgZnCd)S",

abstract = "High entropy metal chalcogenides are an emergent class of materials that have shown exceptional promise in applications such as energy storage, catalysis, and thermoelectric energy conversion. However, the stability of these materials to factors other than temperature are as yet unknown. Here we set out to assess the stability of the high entropy metal sulfide (MnFeCuAgZnCd)S with high pressure (up to 9 GPa), compared to an enthalpically stabilised Ag3CuS2, and a quasi-stable (MnFeZnCd)S. Compression and pressure-annealing of (MnFeCuAgZnCd)S showed diffusion-controlled time and pressure dependent exsolution of jalpaite (Ag3CuS2) from the bulk. Bulk materials characterisation found minor phase impurities and possible elemental localisations in (MnFeCuAgZnCd)S prior to pressure-annealing. To gain deeper understanding of the material pre- and post-pressure annealing at the nanoscale an advanced technique was used which combined machine learning, unsupervised clustering analysis of STEM-EDX mapping with scanning precession electron diffraction (SPED), which revealed a chemically distinct post-pressure annealed jalpaite exsolved from (MnFeCuAgZnCd)S.",

author = "Buckingham, {Mark A.} and Shea, {Joshua J.} and Quan, {Kho Zhi} and Lo, {Pok Man Ethan} and Joshua Swindell and Weichen Xiao and Lewis, {David J.} and Eggeman, {Alex S.} and Hunt, {Simon A.}",

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doi = "10.1038/s42004-025-01463-9",

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T1 - Using high pressure to investigate the stability of a high entropy wurtzite structured (MnFeCuAgZnCd)S

AU - Buckingham, Mark A.

AU - Shea, Joshua J.

AU - Quan, Kho Zhi

AU - Lo, Pok Man Ethan

AU - Swindell, Joshua

AU - Xiao, Weichen

AU - Lewis, David J.

AU - Eggeman, Alex S.

AU - Hunt, Simon A.

PY - 2025/3/5

Y1 - 2025/3/5

N2 - High entropy metal chalcogenides are an emergent class of materials that have shown exceptional promise in applications such as energy storage, catalysis, and thermoelectric energy conversion. However, the stability of these materials to factors other than temperature are as yet unknown. Here we set out to assess the stability of the high entropy metal sulfide (MnFeCuAgZnCd)S with high pressure (up to 9 GPa), compared to an enthalpically stabilised Ag3CuS2, and a quasi-stable (MnFeZnCd)S. Compression and pressure-annealing of (MnFeCuAgZnCd)S showed diffusion-controlled time and pressure dependent exsolution of jalpaite (Ag3CuS2) from the bulk. Bulk materials characterisation found minor phase impurities and possible elemental localisations in (MnFeCuAgZnCd)S prior to pressure-annealing. To gain deeper understanding of the material pre- and post-pressure annealing at the nanoscale an advanced technique was used which combined machine learning, unsupervised clustering analysis of STEM-EDX mapping with scanning precession electron diffraction (SPED), which revealed a chemically distinct post-pressure annealed jalpaite exsolved from (MnFeCuAgZnCd)S.

AB - High entropy metal chalcogenides are an emergent class of materials that have shown exceptional promise in applications such as energy storage, catalysis, and thermoelectric energy conversion. However, the stability of these materials to factors other than temperature are as yet unknown. Here we set out to assess the stability of the high entropy metal sulfide (MnFeCuAgZnCd)S with high pressure (up to 9 GPa), compared to an enthalpically stabilised Ag3CuS2, and a quasi-stable (MnFeZnCd)S. Compression and pressure-annealing of (MnFeCuAgZnCd)S showed diffusion-controlled time and pressure dependent exsolution of jalpaite (Ag3CuS2) from the bulk. Bulk materials characterisation found minor phase impurities and possible elemental localisations in (MnFeCuAgZnCd)S prior to pressure-annealing. To gain deeper understanding of the material pre- and post-pressure annealing at the nanoscale an advanced technique was used which combined machine learning, unsupervised clustering analysis of STEM-EDX mapping with scanning precession electron diffraction (SPED), which revealed a chemically distinct post-pressure annealed jalpaite exsolved from (MnFeCuAgZnCd)S.

U2 - 10.1038/s42004-025-01463-9

DO - 10.1038/s42004-025-01463-9

M3 - Article

SN - 2399-3669

VL - 8

JO - Communications Chemistry

JF - Communications Chemistry

IS - 1

M1 - 65

ER -

Using high pressure to investigate the stability of a high entropy wurtzite structured (MnFeCuAgZnCd)S

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