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

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-06-24 DOI:10.1021/acscatal.5c01591

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

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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.

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介孔无定形高熵氧化膜：解锁增强氧化还原活性

高熵氧化物（HEOs）代表了通过熵稳定固溶体形成催化剂设计的前沿。然而，它们的催化效率受到体积和密度的限制。本研究提出了一种战略方法，通过制造具有最大活性位点利用率的介孔非晶HEO薄膜（MA-HEOF）来解决这一挑战。成功的关键在于通过控制沉积沉淀的几何工程策略，将非晶HEO薄膜限制在介孔通道表面。通过显微镜、x射线和中子技术对MA-HEOF的独特结构进行了分析，并通过同位素研究证实了其表面活化晶格氧的富集和氧化还原活性的增强。此外，MA-HEOF还可以稳定和调节集成贵金属位点的性质，增强其在各种反应中的氧化还原活性。本文提出的方法和见解为在催化和其他领域最大限度地利用高熵材料提供了指导。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.