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

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

doi:10.1021/jacs.4c06423

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

Journal Article · Tue Aug 13 04:00:00 EDT 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.4c06423· OSTI ID:2439858

Liccardo, Gennaro ^[1]; Cendejas, Melissa C. ^[2]; ^[1]; Stone, Michael L. ^[1]; ^[3]; Nhan, Bang T. ^[4]; Kumar, Abinash ^[5]; ^[6]; Plessow, Philipp N. ^[7]; ^[4]; Osio-Norgaard, Jorge ^[1]; ^[8]; ^[9]; ^[3]; ^[1]; ^[1]

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; Stanford Univ., CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Univ. of New Mexico, Albuquerque, NM (United States)
Stanford Univ., CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); North Carolina State University, Raleigh, NC (United States)
Karlsruhe Inst. of Technology (KIT) (Germany)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Duke Univ., Durham, NC (United States)

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. Here, 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 Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725; SC0022197

OSTI ID:: 2439858

Alternate ID(s):: OSTI ID: 2440217

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 34 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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