Chemical Kinetics of Metal Single Atom and Nanocluster Formation on Surfaces: An Example of Pt on Hexagonal Boron Nitride

Popov, Ilya; Ghaderzadeh, Sadegh; Kohlrausch, Emerson C.; Norman, Luke T.; Slater, Thomas J. A.; Aliev, Gazi N.; Alhabeadi, Hanan; Kaplan, Andre; Theis, Wolfgang; Khlobystov, Andrei N.; Fernandes, Jesum Alves; Besley, Elena

Abstract

The production of atomically dispersed metal catalysts remains a significant challenge in the field of heterogeneous catalysis due to coexistence with continuously packed sites such as nanoclusters and nanoparticles. This work presents a comprehensive guidance on how to increase the degree of atomization through a selection of appropriate experimental conditions and supports. It is based on a rigorous macro-kinetic theory that captures relevant competing processes of nucleation and formation of single atoms stabilized by point defects. The effects of metal-support interactions and deposition parameters on the resulting single atom to nanocluster ratio as well as the role of metal centers formed on point defects in the kinetics of nucleation have been established, thus paving the way to guided synthesis of single atom catalysts. The predictions are supported by experimental results on sputter deposition of Pt on exfoliated hexagonal boron nitride, as imaged by aberration-corrected scanning transmission electron microscopy.

Citation

Popov, I., Ghaderzadeh, S., Kohlrausch, E. C., Norman, L. T., Slater, T. J. A., Aliev, G. N., Alhabeadi, H., Kaplan, A., Theis, W., Khlobystov, A. N., Fernandes, J. A., & Besley, E. (2023). Chemical Kinetics of Metal Single Atom and Nanocluster Formation on Surfaces: An Example of Pt on Hexagonal Boron Nitride. Nano Letters, https://doi.org/10.1021/acs.nanolett.3c01968

• Journal Article Type: Letter
• Acceptance Date: Aug 14, 2023
• Online Publication Date: Aug 18, 2023
• Publication Date: Aug 18, 2023
• Deposit Date: Sep 8, 2023
• Publicly Available Date: Sep 11, 2023
• Journal: Nano Letters
• Print ISSN: 1530-6984
• Electronic ISSN: 1530-6992
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• DOI: https://doi.org/10.1021/acs.nanolett.3c01968
• Keywords: Mechanical Engineering; Condensed Matter Physics; General Materials Science; General Chemistry; Bioengineering
• Public URL: https://nottingham-repository.worktribe.com/output/24585699
• Publisher URL: https://pubs.acs.org/doi/10.1021/acs.nanolett.3c01968