High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide

Fluorite-structured oxides constitute an important category of oxides with a wide range of high-temperature applications. Following the concept of high entropy, high-entropy fluorite oxides (HEFOs) have showcased intriguing high-temperature application potential. However, unlocking this potential ne...

Full description

Bibliographic Details
Main Authors: Yixuan Hu, Mariappan Anandkumar, Yumeng Zhang, Joydip Joardar, Atul Suresh Deshpande, Xiaodong Wang, Kolan Madhav Reddy
Format: Article
Language:English
Published: Tsinghua University Press 2024-03-01
Series:Journal of Advanced Ceramics
Subjects:
Online Access:https://www.sciopen.com/article/10.26599/JAC.2024.9220854
_version_ 1797202608040968192
author Yixuan Hu
Mariappan Anandkumar
Yumeng Zhang
Joydip Joardar
Atul Suresh Deshpande
Xiaodong Wang
Kolan Madhav Reddy
author_facet Yixuan Hu
Mariappan Anandkumar
Yumeng Zhang
Joydip Joardar
Atul Suresh Deshpande
Xiaodong Wang
Kolan Madhav Reddy
author_sort Yixuan Hu
collection DOAJ
description Fluorite-structured oxides constitute an important category of oxides with a wide range of high-temperature applications. Following the concept of high entropy, high-entropy fluorite oxides (HEFOs) have showcased intriguing high-temperature application potential. However, unlocking this potential necessitates an assessment of their long-term stability under high-temperature conditions. In this study, we conducted a prolonged heat treatment at 1000 ℃ on typical HEFO, specifically (CeHfZrGdLa)Ox. After 100 h, high-intensity X-ray diffraction (XRD) revealed a transition from a single-phase fluorite to a multi-phase configuration. Further investigation by analytical electron microscoy (AEM) demonstrated that this degradation resulted from facilitated element diffusion and consequent escalating chemical fluctuation at high temperatures, leading to spontaneous segregation and separation of Ce and La elements, forming Ce-rich, La-poor, and La-rich phases. Notably, the La-rich phase spontaneously transformed from a fluorite structure (space group Fm3¯m) to a bixbyite structure (space group Ia3¯) at elevated temperatures, resulting in the appearance of superstructure reflection in XRD profiles and electron diffraction patterns. Despite the intricate phase decomposition, the energy band gap showed minimal variation, suggesting potential property stability of (CeHfZrGdLa)Ox across a broad range of compositions. These findings offer valuable insights into the future applications of HEFOs.
first_indexed 2024-04-24T08:06:08Z
format Article
id doaj.art-76a31f6f8d1848d6840f1af43e7d7c5d
institution Directory Open Access Journal
issn 2226-4108
2227-8508
language English
last_indexed 2024-04-24T08:06:08Z
publishDate 2024-03-01
publisher Tsinghua University Press
record_format Article
series Journal of Advanced Ceramics
spelling doaj.art-76a31f6f8d1848d6840f1af43e7d7c5d2024-04-17T10:37:39ZengTsinghua University PressJournal of Advanced Ceramics2226-41082227-85082024-03-0113331032210.26599/JAC.2024.9220854High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxideYixuan Hu0Mariappan Anandkumar1Yumeng Zhang2Joydip Joardar3Atul Suresh Deshpande4Xiaodong Wang5Kolan Madhav Reddy6School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaDepartment of Materials Science and Metallurgical Engineering, Indian Institute of Technology Hyderabad, Sangareddy 502285, IndiaSchool of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaInternational Advanced Research Centre for Powder Metallurgy and New Materials (ARCI), Hyderabad 500005, IndiaDepartment of Materials Science and Metallurgical Engineering, Indian Institute of Technology Hyderabad, Sangareddy 502285, IndiaSchool of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaSchool of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaFluorite-structured oxides constitute an important category of oxides with a wide range of high-temperature applications. Following the concept of high entropy, high-entropy fluorite oxides (HEFOs) have showcased intriguing high-temperature application potential. However, unlocking this potential necessitates an assessment of their long-term stability under high-temperature conditions. In this study, we conducted a prolonged heat treatment at 1000 ℃ on typical HEFO, specifically (CeHfZrGdLa)Ox. After 100 h, high-intensity X-ray diffraction (XRD) revealed a transition from a single-phase fluorite to a multi-phase configuration. Further investigation by analytical electron microscoy (AEM) demonstrated that this degradation resulted from facilitated element diffusion and consequent escalating chemical fluctuation at high temperatures, leading to spontaneous segregation and separation of Ce and La elements, forming Ce-rich, La-poor, and La-rich phases. Notably, the La-rich phase spontaneously transformed from a fluorite structure (space group Fm3¯m) to a bixbyite structure (space group Ia3¯) at elevated temperatures, resulting in the appearance of superstructure reflection in XRD profiles and electron diffraction patterns. Despite the intricate phase decomposition, the energy band gap showed minimal variation, suggesting potential property stability of (CeHfZrGdLa)Ox across a broad range of compositions. These findings offer valuable insights into the future applications of HEFOs.https://www.sciopen.com/article/10.26599/JAC.2024.9220854high-entropy fluorite oxides (hefos)phase transitionhigh-temperature stabilityelemental segregation
spellingShingle Yixuan Hu
Mariappan Anandkumar
Yumeng Zhang
Joydip Joardar
Atul Suresh Deshpande
Xiaodong Wang
Kolan Madhav Reddy
High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide
Journal of Advanced Ceramics
high-entropy fluorite oxides (hefos)
phase transition
high-temperature stability
elemental segregation
title High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide
title_full High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide
title_fullStr High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide
title_full_unstemmed High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide
title_short High-temperature elemental segregation induced structure degradation in high-entropy fluorite oxide
title_sort high temperature elemental segregation induced structure degradation in high entropy fluorite oxide
topic high-entropy fluorite oxides (hefos)
phase transition
high-temperature stability
elemental segregation
url https://www.sciopen.com/article/10.26599/JAC.2024.9220854
work_keys_str_mv AT yixuanhu hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide
AT mariappananandkumar hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide
AT yumengzhang hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide
AT joydipjoardar hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide
AT atulsureshdeshpande hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide
AT xiaodongwang hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide
AT kolanmadhavreddy hightemperatureelementalsegregationinducedstructuredegradationinhighentropyfluoriteoxide