Atomic Scale Responses of High Entropy Oxides to Redox Environments

Zhennan Huang; Lu Wang; Tangyuan Li; Kartik Venkatraman; Yang He; Felipe Polo-Garzon; Jacob Smith; Yiheng Du; Liangbing Hu; Zili Wu; De En Jiang; Miaofang Chi

doi:10.1021/acs.nanolett.4c02985

Atomic Scale Responses of High Entropy Oxides to Redox Environments

Zhennan Huang, Lu Wang, Tangyuan Li, Kartik Venkatraman, Yang He, Felipe Polo-Garzon, Jacob Smith, Yiheng Du, Liangbing Hu, Zili Wu, De En Jiang, Miaofang Chi

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

Abstract

The potential of high entropy oxides (HEOs) as high-performance energy storage materials and catalysts has been mainly understood through their bulk structures. However, the importance of their surfaces, which may play an even more critical role, remains largely unknown. In this study, we employed advanced scanning transmission electron microscopy to investigate the atomic-scale structural and chemical responses of CeYLaHfTiZrO_x HEOs to high-temperature redox environments. Our observations reveal dynamic elemental and structural reconstructions in the surface of HEOs under different gas environments, contrasting with the high stability of the bulk structure. Notably, the surfaces of HEO particles consistently exhibit abundant oxygen vacancies, regardless of the redox environment. These findings indicate that HEOs offer distinct advantages in facilitating chemical and electrochemical reactions, relying on oxygen vacancies. Our results also suggest that the exceptional performance of HEOs in energy storage applications arises from surface structural and chemical adaptability.

Original language	English
Pages (from-to)	11537-11543
Number of pages	7
Journal	Nano Letters
Volume	24
Issue number	37
DOIs	https://doi.org/10.1021/acs.nanolett.4c02985
State	Published - Sep 18 2024

Funding

This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC0500OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for the United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Acknowledgments Research was sponsored by the US DOE, Office of Science, Office of Basic Energy Sciences (BES), Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. Technique development and data analysis were supported by U.S. DOE Office of Science under Early Career award no. ERKCZ55. Microscopy experiments were conducted at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Liangbing Hu acknowledges the financial support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0023357 and the U.S. Department of Energy, Office of Science Energy Earthshot Initiative as part of the Non-equilibrium Energy Transfer for Efficient Reactions (NEETER) at Oak Ridge National Laboratory under contract #DE-AC05-00OR22725.

Funders	Funder number
U.S. Department of Energy
Office of Science Energy Earthshot Initiative
Office of Science	ERKCZ55
Basic Energy Sciences	DE-SC0023357
Oak Ridge National Laboratory	-AC05-00OR22725

Keywords

atomic scale
high entropy oxide
redox environment
surface response

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10.1021/acs.nanolett.4c02985

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title = "Atomic Scale Responses of High Entropy Oxides to Redox Environments",

abstract = "The potential of high entropy oxides (HEOs) as high-performance energy storage materials and catalysts has been mainly understood through their bulk structures. However, the importance of their surfaces, which may play an even more critical role, remains largely unknown. In this study, we employed advanced scanning transmission electron microscopy to investigate the atomic-scale structural and chemical responses of CeYLaHfTiZrOx HEOs to high-temperature redox environments. Our observations reveal dynamic elemental and structural reconstructions in the surface of HEOs under different gas environments, contrasting with the high stability of the bulk structure. Notably, the surfaces of HEO particles consistently exhibit abundant oxygen vacancies, regardless of the redox environment. These findings indicate that HEOs offer distinct advantages in facilitating chemical and electrochemical reactions, relying on oxygen vacancies. Our results also suggest that the exceptional performance of HEOs in energy storage applications arises from surface structural and chemical adaptability.",

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author = "Zhennan Huang and Lu Wang and Tangyuan Li and Kartik Venkatraman and Yang He and Felipe Polo-Garzon and Jacob Smith and Yiheng Du and Liangbing Hu and Zili Wu and Jiang, {De En} and Miaofang Chi",

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AU - Huang, Zhennan

AU - Wang, Lu

AU - Li, Tangyuan

AU - Venkatraman, Kartik

AU - He, Yang

AU - Polo-Garzon, Felipe

AU - Smith, Jacob

AU - Du, Yiheng

AU - Hu, Liangbing

AU - Wu, Zili

AU - Jiang, De En

AU - Chi, Miaofang

PY - 2024/9/18

Y1 - 2024/9/18

N2 - The potential of high entropy oxides (HEOs) as high-performance energy storage materials and catalysts has been mainly understood through their bulk structures. However, the importance of their surfaces, which may play an even more critical role, remains largely unknown. In this study, we employed advanced scanning transmission electron microscopy to investigate the atomic-scale structural and chemical responses of CeYLaHfTiZrOx HEOs to high-temperature redox environments. Our observations reveal dynamic elemental and structural reconstructions in the surface of HEOs under different gas environments, contrasting with the high stability of the bulk structure. Notably, the surfaces of HEO particles consistently exhibit abundant oxygen vacancies, regardless of the redox environment. These findings indicate that HEOs offer distinct advantages in facilitating chemical and electrochemical reactions, relying on oxygen vacancies. Our results also suggest that the exceptional performance of HEOs in energy storage applications arises from surface structural and chemical adaptability.

AB - The potential of high entropy oxides (HEOs) as high-performance energy storage materials and catalysts has been mainly understood through their bulk structures. However, the importance of their surfaces, which may play an even more critical role, remains largely unknown. In this study, we employed advanced scanning transmission electron microscopy to investigate the atomic-scale structural and chemical responses of CeYLaHfTiZrOx HEOs to high-temperature redox environments. Our observations reveal dynamic elemental and structural reconstructions in the surface of HEOs under different gas environments, contrasting with the high stability of the bulk structure. Notably, the surfaces of HEO particles consistently exhibit abundant oxygen vacancies, regardless of the redox environment. These findings indicate that HEOs offer distinct advantages in facilitating chemical and electrochemical reactions, relying on oxygen vacancies. Our results also suggest that the exceptional performance of HEOs in energy storage applications arises from surface structural and chemical adaptability.

KW - atomic scale

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KW - redox environment

KW - surface response

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Atomic Scale Responses of High Entropy Oxides to Redox Environments

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