Atomic‐Scale Insights into Nanoparticle Exsolution at Dislocations in Dislocation‐Engineered Catalysts

Advanced Materials, vol. 38, pp. e02362

Abstract

Achieving control over properties such as density and lateral distribution of catalytic nanoparticles under operation conditions is a major challenge for the development of active and durable catalysts, where nanoparticle coarsening is often the cause of performance degradation. While metal exsolution catalysts are regarded to be robust against this degradation mode, coarsening and increased concentrations of exsolved metal nanoparticles have been detected near extended defects. The present study examines the role of dislocations in metal exsolution reactions and explores the potential of dislocation-engineering for the synthesis of dislocation-associated nanoparticles. An atomic-level correlation between bulk dislocations and surface nanoparticle locations is demonstrated through a novel approach for engineering epitaxial thin films with confined regions of increased dislocation densities in combination with in situ scanning transmission electron microscopy. While nanoparticle exsolution proceeds across the entire sample, two primary reasons for the frequent nucleation of dislocation-associated nanoparticles are identified: the accumulation of exsolution-active acceptors along dislocations and lattice distortions that are likely to lower the energy barrier for nanoparticle nucleation. This work establishes a proof of concept for using engineered dislocations in exsolution catalysts to synthesize nanoparticles with modified nanoparticle-support properties relevant for the thermal stability and the lateral distribution of exsolved nanoparticles.

Authors 9

1. Moritz Lukas Weber corresponding

   Kyushu University · Forschungszentrum Jülich · Massachusetts Institute of Technology

   Affiliation as printed

   Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA

   Next‐Generation Fuel Cell Research Center Kyushu University 744 Motooka Nishi‐ku Fukuoka 819‐0395 Japan

   Peter Grünberg Institute Electronic Materials (PGI‐7) Forschungszentrum Jülich GmbH 52425 Jülich Germany

   Next-Generation Fuel Cell Research Center, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka, 819-0395 Japan

   Peter Grünberg Institute, Electronic Materials (PGI-7), Forschungszentrum Jülich GmbH, 52425, Jülich, Germany

2. Moritz Kindelmann corresponding

   Forschungszentrum Jülich · Ernst Ruska Centre

   Affiliation as printed

   Ernst Ruska‐Centre for Microscopy and Spectroscopy with Electrons (ER‐C) Forschungszentrum Jülich GmbH 52425 Jülich Germany

   Institute of Energy Materials and Devices Materials Synthesis and Processing (IMD‐2) Forschungszentrum Jülich GmbH 52425 Jülich Germany

3. Dylan Jennings corresponding

   University of Stuttgart · Forschungszentrum Jülich · Ernst Ruska Centre

   Affiliation as printed

   Ernst Ruska‐Centre for Microscopy and Spectroscopy with Electrons (ER‐C) Forschungszentrum Jülich GmbH 52425 Jülich Germany

   Institute for Manufacturing Technologies of Ceramic Components and Composites University of Stuttgart 70569 Stuttgart Germany

   Institute of Energy Materials and Devices Materials Synthesis and Processing (IMD‐2) Forschungszentrum Jülich GmbH 52425 Jülich Germany

4. Jan Hölschke

   Technische Universität Darmstadt

   Affiliation as printed

   Department of Materials and Earth Sciences Technical University of Darmstadt 64287 Darmstadt Germany

   Department of Materials and Earth Sciences, Technical University of Darmstadt, 64287 Darmstadt, Germany

5. Regina Dittmann

   Forschungszentrum Jülich

   Affiliation as printed

   Peter Grünberg Institute Electronic Materials (PGI‐7) Forschungszentrum Jülich GmbH 52425 Jülich Germany

6. Joachim Mayer Aachen Central Facility for Electron Microscopy

   Forschungszentrum Jülich · Ernst Ruska Centre · RWTH Aachen University

   Affiliation as printed

   Central Facility for Electron Microscopy (GFE) RWTH Aachen University 52064 Aachen Germany

   Ernst Ruska‐Centre for Microscopy and Spectroscopy with Electrons (ER‐C) Forschungszentrum Jülich GmbH 52425 Jülich Germany

   Ernst Ruska‐Centre for Microscopy and Spectroscopy with Electrons (ER‐C) Forschungszentrum Jülich GmbH 52425 Jülich Germany

7. Wolfgang Rheinheimer

   University of Stuttgart

   Affiliation as printed

   Institute for Manufacturing Technologies of Ceramic Components and Composites University of Stuttgart 70569 Stuttgart Germany

   Institute for Manufacturing Technologies of Ceramic Components and Composites, University of Stuttgart, 70569 Stuttgart, Germany

8. Xufei Fang corresponding

   Karlsruhe Institute of Technology

   Affiliation as printed

   Institute for Applied Materials Karlsruhe Institute of Technology 76131 Karlsruhe Germany

   Institute for Applied Materials, Karlsruhe Institute of Technology, 76131 Karlsruhe, Germany

   Institute for Applied Materials, Karlsruhe Institute of Technology, 76131, Karlsruhe, Germany

9. Felix Gunkel corresponding

   Forschungszentrum Jülich

   Affiliation as printed

   Peter Grünberg Institute Electronic Materials (PGI‐7) Forschungszentrum Jülich GmbH 52425 Jülich Germany