Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition

Gennaro Liccardo; Melissa C. Cendejas; Shyama C. Mandal; Michael L. Stone; Stephen Porter; Bang T. Nhan; Abinash Kumar; Jacob Smith; Philipp N. Plessow; Lynette Cegelski; Jorge Osio-Norgaard; Frank Abild-Pedersen; Miaofang Chi; Abhaya K. Datye; Stacey F. Bent; Matteo Cargnello

doi:10.1021/jacs.4c06423

Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition

Gennaro Liccardo, Melissa C. Cendejas, Shyama C. Mandal, Michael L. Stone, Stephen Porter, Bang T. Nhan, Abinash Kumar, Jacob Smith, Philipp N. Plessow, Lynette Cegelski, Jorge Osio-Norgaard, Frank Abild-Pedersen, Miaofang Chi, Abhaya K. Datye, Stacey F. Bent, Matteo Cargnello

electron Microscopy and Microanalysis

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

2 Scopus citations

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.

Original language	English
Pages (from-to)	23909-23922
Number of pages	14
Journal	Journal of the American Chemical Society
Volume	146
Issue number	34
DOIs	https://doi.org/10.1021/jacs.4c06423
State	Published - Aug 28 2024

Funding

G.L. acknowledges Simon R. Bare for his support throughout this project. This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-SC0022197. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-2026822. L.C. acknowledges support from the National Science Foundation Award no. 2001189. P.N.P. acknowledges funding by Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)\u2500SFB 1441\u2500Project ID 426888090. M.L.S. acknowledges support from a TomKat Postdoctoral Fellowship in Sustainable Energy from the TomKat Center at Stanford University. Electron microscopy was performed at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory.

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10.1021/jacs.4c06423

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Liccardo, G., Cendejas, M. C., Mandal, S. C., Stone, M. L., Porter, S., Nhan, B. T., Kumar, A., Smith, J., Plessow, P. N., Cegelski, L., Osio-Norgaard, J., Abild-Pedersen, F., Chi, M., Datye, A. K., Bent, S. F., & Cargnello, M. (2024). Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition. Journal of the American Chemical Society, 146(34), 23909-23922. https://doi.org/10.1021/jacs.4c06423

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title = "Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition",

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.",

author = "Gennaro Liccardo and Cendejas, {Melissa C.} and Mandal, {Shyama C.} and Stone, {Michael L.} and Stephen Porter and Nhan, {Bang T.} and Abinash Kumar and Jacob Smith and Plessow, {Philipp N.} and Lynette Cegelski and Jorge Osio-Norgaard and Frank Abild-Pedersen and Miaofang Chi and Datye, {Abhaya K.} and Bent, {Stacey F.} and Matteo Cargnello",

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Liccardo, G, Cendejas, MC, Mandal, SC, Stone, ML, Porter, S, Nhan, BT, Kumar, A, Smith, J, Plessow, PN, Cegelski, L, Osio-Norgaard, J, Abild-Pedersen, F, Chi, M, Datye, AK, Bent, SF & Cargnello, M 2024, 'Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition', Journal of the American Chemical Society, vol. 146, no. 34, pp. 23909-23922. https://doi.org/10.1021/jacs.4c06423

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T1 - Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition

AU - Liccardo, Gennaro

AU - Cendejas, Melissa C.

AU - Mandal, Shyama C.

AU - Stone, Michael L.

AU - Porter, Stephen

AU - Nhan, Bang T.

AU - Kumar, Abinash

AU - Smith, Jacob

AU - Plessow, Philipp N.

AU - Cegelski, Lynette

AU - Osio-Norgaard, Jorge

AU - Abild-Pedersen, Frank

AU - Chi, Miaofang

AU - Datye, Abhaya K.

AU - Bent, Stacey F.

AU - Cargnello, Matteo

PY - 2024/8/28

Y1 - 2024/8/28

N2 - 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.

AB - 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.

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U2 - 10.1021/jacs.4c06423

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AN - SCOPUS:85201405900

SN - 0002-7863

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SP - 23909

EP - 23922

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 34

ER -

Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition

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