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.
(2023) Journal of the American Chemical Society, volume 145, issue 31, pp. 17299 - 17308
(Article)
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
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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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Keywords: Hydrogenation, Nanocatalysts, Methane, Silica, General Chemistry, Biochemistry, Catalysis, Colloid and Surface Chemistry
ISSN: 0002-7863
Publisher: American Chemical Society
Note: Funding Information: Our appreciation goes to Florian Meirer (Utrecht University, UU) for input in the XAS data processing and Kordula B. Schnabl (UU) for scientific discussions. We also thank Floris D. van Oort (UU) for his technical support in performing the resin impregnation. Furthermore, we are very grateful for the contributions of Joren M. Dorresteijn (in measuring the SEM-EDX data, UU) and Ali Kosari (in measuring the STEM-EDX data, UU). This work is part of the Advanced Research Center for Chemical Building Blocks, ARC CBBC, which is cofounded and cofinanced by the Dutch Research Council (NWO) and The Netherlands Ministry of Economic Affairs and Climate Policy. The APT research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility, at Oak Ridge National Laboratory. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.
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