Title: Elucidating the Structure and Composition of Individual Bimetallic Nanoparticles in Supported Catalysts by Atom Probe Tomography

Abstract

Understanding and controlling the structure and composition of nanoparticles in supported metal catalysts are crucial to improve chemical processes. For this, atom probe tomography (APT) is a unique tool, as it allows for spatially resolved three-dimensional chemical imaging of materials with sub-nanometer resolution. However, thus far APT has not been applied for mesoporous oxide-supported metal catalyst materials, due to the size and number of pores resulting in sample fracture during experiments. To overcome these issues, we developed a high-pressure resin impregnation strategy and showcased the applicability to high-porous supported Pd–Ni-based catalyst materials, which are active in CO2 hydrogenation. Within the reconstructed volume of 3 × 105 nm3, we identified over 400 Pd–Ni clusters, with compositions ranging from 0 to 16 atom % Pd and a size distribution of 2.6 ± 1.6 nm. These results illustrate that APT is capable of quantitatively assessing the size, composition, and metal distribution for a large number of nanoparticles at the sub-nm scale in industrial catalysts. Furthermore, we showcase that metal segregation occurred predominately between nanoparticles, shedding light on the mechanism of metal segregation. We envision that the presented methodology expands the capabilities of APT to investigate porous functional nanomaterials, including but not limited tomore » solid catalysts.« less

Authors:

Zand, Florian  ^[1];

• Search DOE PAGES for author "Zand, Florian"
• Search DOE PAGES for ORCID "0000-0002-9153-1610"

Hangx, Suzanne J. T. ^[2]; Spiers, Christopher J. ^[2]; van den Brink, Peter J. ^[3]; Burns, James ^[4]; Boebinger, Matthew G. ^[4]; Poplawsky, Jonathan D.  ^[4];

• Search DOE PAGES for author "Poplawsky, Jonathan D."
• Search DOE PAGES for ORCID "0000-0002-4272-7043"

Monai, Matteo  ^[1];

• Search DOE PAGES for author "Monai, Matteo"
• Search DOE PAGES for ORCID "0000-0001-6945-4391"

Weckhuysen, Bert M.  ^[1]

• Search DOE PAGES for author "Weckhuysen, Bert M."
• Search DOE PAGES for ORCID "0000-0001-5245-1426"

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+ Show Author Affiliations

1. Inorganic Chemistry and Catalysis Group, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University, 3584 CG Utrecht, The Netherlands
2. High Pressure and Temperature Laboratory, Utrecht University, 3584 CB Utrecht, The Netherlands
3. Shell Global Solutions, 1031 HW Amsterdam, The Netherlands
4. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States

Publication Date:

Tue Jul 25 00:00:00 EDT 2023

Research Org.:

Utrecht University (Netherlands); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Org.:

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

OSTI Identifier:

1992384

Alternate Identifier(s):

OSTI ID: 1994271; OSTI ID: 1996638

Grant/Contract Number:  

AC05-00OR22725

Resource Type:

Published Article

Journal Name:

Journal of the American Chemical Society

Additional Journal Information:

Journal Name: Journal of the American Chemical Society Journal Volume: 145 Journal Issue: 31; Journal ID: ISSN 0002-7863

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysts; cluster chemistry; metals; nanoparticles; palladium