Mesoporous Amorphous High-Entropy Oxide Films: Unlocking Enhanced Redox Activity

Qingju Wang; Meijia Li; Kevin M. Siniard; Darren M. Driscoll; Alexander S. Ivanov; Jue Liu; Shize Yang; Junyan Zhang; Felipe Polo-Garzon; Austin Houston; Gerd Duscher; Zhenzhen Yang; Sheng Dai

doi:10.1021/acscatal.5c01591

Mesoporous Amorphous High-Entropy Oxide Films: Unlocking Enhanced Redox Activity

Qingju Wang, Meijia Li, Kevin M. Siniard, Darren M. Driscoll, Alexander S. Ivanov, Jue Liu, Shize Yang, Junyan Zhang, Felipe Polo-Garzon, Austin Houston, Gerd Duscher, Zhenzhen Yang, Sheng Dai

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

Abstract

High-entropy oxides (HEOs) represent a frontier in catalyst design via entropy-stabilized solid solution formation. However, their catalytic efficiency is limited by their bulk and dense nature. This work presents a strategic approach to tackle this challenge by fabricating mesoporous amorphous HEO films (MA-HEOF) possessing maximized active site utilization efficiency. The success hinges on the as-developed geometric engineering strategy via controlled deposition-precipitation to confine the amorphous HEO thin film on the surface of mesoporous channels. The unique structure of MA-HEOF was elucidated via microscopy-, X-ray-, and neutron-based techniques, which were manifested by enriched surface-activated lattice oxygen and enhanced redox activity, as confirmed by isotope studies. Besides, the MA-HEOF could stabilize and modulate the properties of integrated noble metal sites, enhancing their redox activity in diverse reactions. The approaches and insights presented herein provide guidance on maximizing the utilization efficiency of high-entropy materials in catalysis and beyond.

Original language	English
Pages (from-to)	11806-11817
Number of pages	12
Journal	ACS Catalysis
Volume	15
Issue number	13
DOIs	https://doi.org/10.1021/acscatal.5c01591
State	Published - Jul 4 2025

Funding

The research was supported financially by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. Use of the NSLS-II (NIST beamline 6-BM and the 28-ID-1 beamline) was supported by the Department of Energy Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory (BNL) under contract no. DE-SC0012704. D.M.D. and A.S.I. thank Dr. Ravel and Dr. Kwon of BNL for their help during synchrotron experiments. Neutron total scattering measurements were conducted at the NOMAD beamline at the Spallation Neutron Source, Oak Ridge National Laboratory, which was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, U.S. Department of Energy. Scanning transmission electron microscopy characterization was performed at the Institute for Advanced Materials and Manufacturing (IAMM), University of Tennessee, Knoxville.

Keywords

heterogeneous catalysis
high-entropy oxide
hydrogenation
mesoporous material
surface confinement

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10.1021/acscatal.5c01591

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title = "Mesoporous Amorphous High-Entropy Oxide Films: Unlocking Enhanced Redox Activity",

abstract = "High-entropy oxides (HEOs) represent a frontier in catalyst design via entropy-stabilized solid solution formation. However, their catalytic efficiency is limited by their bulk and dense nature. This work presents a strategic approach to tackle this challenge by fabricating mesoporous amorphous HEO films (MA-HEOF) possessing maximized active site utilization efficiency. The success hinges on the as-developed geometric engineering strategy via controlled deposition-precipitation to confine the amorphous HEO thin film on the surface of mesoporous channels. The unique structure of MA-HEOF was elucidated via microscopy-, X-ray-, and neutron-based techniques, which were manifested by enriched surface-activated lattice oxygen and enhanced redox activity, as confirmed by isotope studies. Besides, the MA-HEOF could stabilize and modulate the properties of integrated noble metal sites, enhancing their redox activity in diverse reactions. The approaches and insights presented herein provide guidance on maximizing the utilization efficiency of high-entropy materials in catalysis and beyond.",

keywords = "heterogeneous catalysis, high-entropy oxide, hydrogenation, mesoporous material, surface confinement",

author = "Qingju Wang and Meijia Li and Siniard, \{Kevin M.\} and Driscoll, \{Darren M.\} and Ivanov, \{Alexander S.\} and Jue Liu and Shize Yang and Junyan Zhang and Felipe Polo-Garzon and Austin Houston and Gerd Duscher and Zhenzhen Yang and Sheng Dai",

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doi = "10.1021/acscatal.5c01591",

language = "English",

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TY - JOUR

T1 - Mesoporous Amorphous High-Entropy Oxide Films

T2 - Unlocking Enhanced Redox Activity

AU - Wang, Qingju

AU - Li, Meijia

AU - Siniard, Kevin M.

AU - Driscoll, Darren M.

AU - Ivanov, Alexander S.

AU - Liu, Jue

AU - Yang, Shize

AU - Zhang, Junyan

AU - Polo-Garzon, Felipe

AU - Houston, Austin

AU - Duscher, Gerd

AU - Yang, Zhenzhen

AU - Dai, Sheng

PY - 2025/7/4

Y1 - 2025/7/4

N2 - High-entropy oxides (HEOs) represent a frontier in catalyst design via entropy-stabilized solid solution formation. However, their catalytic efficiency is limited by their bulk and dense nature. This work presents a strategic approach to tackle this challenge by fabricating mesoporous amorphous HEO films (MA-HEOF) possessing maximized active site utilization efficiency. The success hinges on the as-developed geometric engineering strategy via controlled deposition-precipitation to confine the amorphous HEO thin film on the surface of mesoporous channels. The unique structure of MA-HEOF was elucidated via microscopy-, X-ray-, and neutron-based techniques, which were manifested by enriched surface-activated lattice oxygen and enhanced redox activity, as confirmed by isotope studies. Besides, the MA-HEOF could stabilize and modulate the properties of integrated noble metal sites, enhancing their redox activity in diverse reactions. The approaches and insights presented herein provide guidance on maximizing the utilization efficiency of high-entropy materials in catalysis and beyond.

AB - High-entropy oxides (HEOs) represent a frontier in catalyst design via entropy-stabilized solid solution formation. However, their catalytic efficiency is limited by their bulk and dense nature. This work presents a strategic approach to tackle this challenge by fabricating mesoporous amorphous HEO films (MA-HEOF) possessing maximized active site utilization efficiency. The success hinges on the as-developed geometric engineering strategy via controlled deposition-precipitation to confine the amorphous HEO thin film on the surface of mesoporous channels. The unique structure of MA-HEOF was elucidated via microscopy-, X-ray-, and neutron-based techniques, which were manifested by enriched surface-activated lattice oxygen and enhanced redox activity, as confirmed by isotope studies. Besides, the MA-HEOF could stabilize and modulate the properties of integrated noble metal sites, enhancing their redox activity in diverse reactions. The approaches and insights presented herein provide guidance on maximizing the utilization efficiency of high-entropy materials in catalysis and beyond.

KW - heterogeneous catalysis

KW - high-entropy oxide

KW - hydrogenation

KW - mesoporous material

KW - surface confinement

UR - https://www.scopus.com/pages/publications/105009081479

U2 - 10.1021/acscatal.5c01591

DO - 10.1021/acscatal.5c01591

M3 - Article

AN - SCOPUS:105009081479

SN - 2155-5435

VL - 15

SP - 11806

EP - 11817

JO - ACS Catalysis

JF - ACS Catalysis

IS - 13

ER -

Mesoporous Amorphous High-Entropy Oxide Films: Unlocking Enhanced Redox Activity

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