Tuning Point Defects by Elastic Strain Modulates Nanoparticle Exsolution on Perovskite Oxides

Wang, Jiayue; Yang, Jing; Opitz, Alexander K.; Bowman, William; Bliem, Roland; Dimitrakopoulos, Georgios; Nenning, Andreas; Waluyo, Iradwikanari; Hunt, Adrian; Gallet, Jean-Jacques; Yildiz, Bilge

doi:10.1021/acs.chemmater.1c00821

Tuning Point Defects by Elastic Strain Modulates Nanoparticle Exsolution on Perovskite Oxides

Journal Article · Tue Jun 15 04:00:00 EDT 2021 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c00821· OSTI ID:1807942

^[1]; ^[1]; ^[2]; ^[1]; ^[3]; ^[1]; Nenning, Andreas ^[4]; ^[5]; Hunt, Adrian ^[5]; Gallet, Jean-Jacques ^[6]; ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Technische Univ. Wien, Austria (Austria)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. of Amsterdam (Netherlands)
Technische Univ. Wien, Austria (Austria)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sorbonne Univ., Paris (France); Synchrotron SOLEIL, Gif-sur-Yvette (France)

Exsolution generates stable and catalytically active metal nanoparticles via phase precipitation out of a host oxide. An ability to control the size and dispersion of the exsolution particles is desirable for design of nanostructured (electro)catalysts. In this work, we demonstrate that tuning point defects by lattice strain affects both the thermodynamics and the kinetics of iron (Fe⁰) exsolution on La^0.6Sr^0.4FeO³ (LSF) thin film model. By combining in situ surface characterization and ab initio defect modeling, we show oxygen vacancy and Schottky defects to be the primary point defects formed upon Fe0 exsolution. Lattice strain tunes the formation energy, and thus the abundance of these defects, and alters the amount and size of the resulting exsolution particles. In addition, we find that the density of exsolved nanoparticles matches the concentration of oxygen vacancy pairs, thus pointing to the surface oxygen vacancy pairs as preferential nucleation sites for exsolution. The tensile-strained LSF with a facile formation of these critical point defects results in a higher Fe⁰ metal concentration, a larger density of nanoparticles, and a reduced particle size at its surfaces. These results provide important mechanistic insights and highlight the role of point-defect engineering in designing nanostructured catalysts in energy and fuel conversion technologies.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1807942

Report Number(s):: BNL--221797-2021-JAAM

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 13 Vol. 33; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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