Bang T Nhan
Ph.D. Student in Chemistry, admitted Autumn 2021
All Publications
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A General Approach for Metal Nanoparticle Encapsulation Within Porous Oxides.
Advanced materials (Deerfield Beach, Fla.)
2024: e2409710
Abstract
Encapsulation of metal nanoparticles within oxide materials has been shown as an effective strategy to improve activity, selectivity, and stability in several catalytic applications. Several approaches have been proposed to encapsulate nanoparticles, such as forming core-shell structures, growing ordered structures (zeolites or metal-organic frameworks) on nanoparticles, or directly depositing support materials on nanoparticles. Here, a general nanocasting method is demonstrated that can produce diverse encapsulated metal@oxide structures with different compositions (Pt, Pd, Rh) and multiple types of oxides (Al2O3, Al2O3-CeO2, ZrO2, ZnZrOx, In2O3, Mn2O3, TiO2) while controlling the size and dispersion of nanoparticles and the porous structure of the oxide. Metal@polymer structures are first prepared, and then the oxide precursor is infiltrated into such structures and the resulting material is calcined to form the metal@oxide structures. Most Pt@oxides catalysts show similar catalytic activity, demonstrating the availability of surface Pt sites in the encapsulated structures. However, the Pt@Mn2O3 sample showed much higher CO oxidation activity, while also being stable under aging conditions. This work demonstrated a robust nanocasting method to synthesize metal@oxide structures, which can be utilized in catalysis to finely tune metal-oxide interfaces.
View details for DOI 10.1002/adma.202409710
View details for PubMedID 39523738
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Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition.
Journal of the American Chemical Society
2024
Abstract
Platinum exhibits desirable catalytic properties, but it is scarce and expensive. Optimizing its use in key applications such as emission control catalysis is important to reduce our reliance on such a rare element. Supported Pt nanoparticles (NPs) used in emission control systems deactivate over time because of particle growth in sintering processes. In this work, we shed light on the stability against sintering of Pt NPs supported on and encapsulated in Al2O3 using a combination of nanocrystal catalysts and atomic layer deposition (ALD) techniques. We find that small amounts of alumina overlayers created by ALD on preformed Pt NPs can stabilize supported Pt catalysts, significantly reducing deactivation caused by sintering, as previously observed by others. Combining theoretical and experimental insights, we correlate this behavior to the decreased propensity of oxidized Pt species to undergo Ostwald ripening phenomena because of the physical barrier imposed by the alumina overlayers. Furthermore, we find that highly stable catalysts can present an abundance of under-coordinated Pt sites after restructuring of both Pt particles and alumina overlayers at a high temperature (800 °C) in C3H6 oxidation conditions. The enhanced stability significantly improves the Pt utilization efficiency after accelerated aging treatments, with encapsulated Pt catalysts reaching reaction rates more than two times greater than those of a control supported Pt catalyst.
View details for DOI 10.1021/jacs.4c06423
View details for PubMedID 39137357