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

Zand, Florian; Hangx, Suzanne J. T.; Spiers, Christopher J.; van den Brink, Peter J.; Burns, James; Boebinger, Matthew G.; Poplawsky, Jonathan D.; Monai, Matteo; Weckhuysen, Bert M.

doi:10.1021/jacs.3c04474

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

Journal Article · Tue Jul 25 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c04474· OSTI ID:1992384

^[1]; Hangx, Suzanne J. T. ^[2]; Spiers, Christopher J. ^[2]; van den Brink, Peter J. ^[3]; Burns, James ^[4]; Boebinger, Matthew G. ^[4];

^[4];

^[1];

^[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
High Pressure and Temperature Laboratory, Utrecht University, 3584 CB Utrecht, The Netherlands
Shell Global Solutions, 1031 HW Amsterdam, The Netherlands
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States

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 to solid catalysts.

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

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1992384

Alternate ID(s):: OSTI ID: 1994271; OSTI ID: 1996638

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Vol. 145 Journal Issue: 31; ISSN 0002-7863

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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