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1.
J Am Chem Soc ; 146(34): 23909-23922, 2024 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-39137357

RESUMO

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.

2.
ACS Appl Mater Interfaces ; 11(46): 43337-43343, 2019 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-31647628

RESUMO

Efficient removal of CO2 from enclosed environments is a significant challenge, particularly in human space flight where strict restrictions on mass and volume are present. To address this issue, this study describes the use of a multimaterial, layer-by-layer, additive manufacturing technique to directly print a structured multifunctional composite for CO2 sorption with embedded, intrinsic, heating capability to facilitate thermal desorption, removing the need for an external heat source from the system. This multifunctional composite is coprinted from an ink formulation based on zeolite 13X, and an electrically conductive sorbent ink formulation, which includes metal particles blended with the zeolite. The composites are characterized using analytical and imaging tools and then tested for CO2 adsorption/desorption. The resistivity of the conductive sorbent is <2 mΩ m, providing a temperature increase up to 200 °C under 7 V applied bias, which is sufficient to trigger CO2 desorption. The CO2 adsorption capability of the conductive zeolite ink appears to be unaffected by the presence of the conductive particles, meaning a large fraction of the total mass of the structured composite device is functional.

3.
Materials (Basel) ; 12(12)2019 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-31238498

RESUMO

This work presents experimental evidence that confirms the potential for two specific zeolites, namely chabazite and faujasite (with a cage size ~2-13 Å), to adsorb small amounts of chloride from a synthetic alkali-activated cement (AAC) pore solution. Four synthetic zeolites were first exposed to a chlorinated AAC pore solution, two faujasite zeolites (i.e., FAU, X-13), chabazite (i.e., SSZ-13), and sodium-stabilized mordenite (i.e., Na-Mordenite). The mineralogy and chemical composition were subsequently investigated via X-ray diffraction (XRD) and both energy- and wavelength-dispersive X-ray spectroscopy (WDS), respectively. Upon exposure to a chlorinated AAC pore solution, FAU and SSZ-13 displayed changes to their diffraction patterns (i.e., peak shifting and broadening), characteristic of ion entrapment within zeolitic aluminosilicate frameworks. Elemental mapping with WDS confirmed the presence of small amounts of elemental chlorine. Results indicate that the chloride-bearing capacity of zeolites is likely dependent on both microstructural features (e.g., cage sizes) and chemical composition.

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