Thermal stability and coalescence dynamics of exsolved metal nanoparticles at charged perovskite surfaces

Weber, Moritz L.; Jennings, Dylan; Fearn, Sarah; Cavallaro, Andrea; Prochazka, Michal; Gutsche, Alexander; Heymann, Lisa; Guo, Jia; Yasin, Liam; Cooper, Samuel J.; Mayer, Joachim; Rheinheimer, Wolfgang; Dittmann, Regina; Waser, Rainer; Guillon, Olivier; Lenser, Christian; Skinner, Stephen J.; Aguadero, Ainara; Nemšák, Slavomír; Gunkel, Felix

doi:10.1038/s41467-024-54008-4

Title: Thermal stability and coalescence dynamics of exsolved metal nanoparticles at charged perovskite surfaces

Journal Article · 08 November 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-54008-4 · OSTI ID:2481715

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Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Imperial College, London (United Kingdom); Forschungszentrum Juelich (Germany). Peter Gruenberg Institute for Electronic Materials (PGI-7) and Juelich-Aachen Research Alliance (JARA-FIT); Forschungszentrum Juelich (Germany). Materials Synthesis and Processing (IMD-2); Kyushu Univ., Fukuoka (Japan)
Forschungszentrum Juelich (Germany). Materials Synthesis and Processing (IMD-2) and Materials Science and Technology (ER-C 2); Univ. of Stuttgart (Germany)
Imperial College, London (United Kingdom)
Imperial College, London (United Kingdom); University of Bergamo, Dalmine (Italy)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); University of West Bohemia, Pilsen (Czech Republic)
Forschungszentrum Juelich (Germany). Peter Gruenberg Institute for Electronic Materials (PGI-7) and Juelich-Aachen Research Alliance (JARA-FIT)
Forschungszentrum Juelich (Germany). Materials Science and Technology (ER-C 2); RWTH Aachen Univ. (Germany)
Forschungszentrum Juelich (Germany). Materials Synthesis and Processing (IMD-2); Univ. of Stuttgart (Germany)
Forschungszentrum Juelich (Germany). Peter Gruenberg Institute for Electronic Materials (PGI-7) and Juelich-Aachen Research Alliance (JARA-FIT); RWTH Aachen Univ. (Germany)
Forschungszentrum Juelich (Germany). Materials Synthesis and Processing (IMD-2); RWTH Aachen Univ. (Germany); Juelich-Aachen Research Alliance (JARA-Energy), Juelich (Germany)
Forschungszentrum Juelich (Germany). Materials Synthesis and Processing (IMD-2)
Imperial College, London (United Kingdom); Consejo Superior de Investigaciones Cientificas (CSIC), Madrid (Spain). Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Davis, CA (United States)

Exsolution reactions enable the synthesis of oxide-supported metal nanoparticles, which are desirable as catalysts in green energy conversion technologies. It is crucial to precisely tailor the nanoparticle characteristics to optimize the catalysts’ functionality, and to maintain the catalytic performance under operation conditions. We use chemical (co)-doping to modify the defect chemistry of exsolution-active perovskite oxides and examine its influence on the mass transfer kinetics of Ni dopants towards the oxide surface and on the subsequent coalescence behavior of the exsolved nanoparticles during a continuous thermal reduction treatment. Nanoparticles that exsolve at the surface of the acceptor-type fast-oxygen-ion-conductor SrTi_0.95Ni_0.05O_3–δ (STNi) show a high surface mobility leading to a very low thermal stability compared to nanoparticles that exsolve at the surface of donor-type SrTi_0.9Nb_0.05Ni_0.05O_3–δ (STNNi). Our analysis indicates that the low thermal stability of exsolved nanoparticles at the acceptor-doped perovskite surface is linked to a high oxygen vacancy concentration at the nanoparticle-oxide interface. For catalysts that require fast oxygen exchange kinetics, exsolution synthesis routes in dry hydrogen conditions may hence lead to accelerated degradation, while humid reaction conditions may mitigate this failure mechanism.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2481715

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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