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

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

doi:10.1021/acs.nanolett.3c01968

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

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

^*Corresponding author for this work

Physics and Astronomy

Research output: Contribution to journal › Letter › peer-review

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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.

Original language	English
Pages (from-to)	8006-8012
Number of pages	7
Journal	Nano Letters
Volume	23
Issue number	17
Early online date	18 Aug 2023
DOIs	https://doi.org/10.1021/acs.nanolett.3c01968
Publication status	Published - 13 Sept 2023

Bibliographical note

Acknowledgments:
This work was funded by the Engineering and Physical Sciences Research Council (EPSRC) Programme Grant ‘Metal Atoms on Surfaces and Interfaces (MASI) for Sustainable Future’ (EP/V000055/1). E.B. acknowledges a Royal Society Wolfson Fellowship for financial support.

Keywords

single atom catalysts
point defects in 2D materials
nucleation kinetics
metal nanoclusters

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10.1021/acs.nanolett.3c01968Licence: Creative Commons: Attribution (CC BY)

PopovI2023ChemicalFinal published version, 5.61 MBLicence: Creative Commons: Attribution (CC BY)

https://pubs.acs.org/doi/10.1021/acs.nanolett.3c01968Licence: Creative Commons: Attribution (CC BY)

Metal Atoms on Surfaces & Interfaces (MASI) for Sustainable Future
Theis, W. & Rees, N.
Engineering & Physical Science Research Council
1/08/21 → 31/07/26
Project: Research Councils

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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, 23(17), 8006-8012. https://doi.org/10.1021/acs.nanolett.3c01968

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

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.",

keywords = "single atom catalysts, point defects in 2D materials, nucleation kinetics, metal nanoclusters",

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

note = "Acknowledgments: This work was funded by the Engineering and Physical Sciences Research Council (EPSRC) Programme Grant {\textquoteleft}Metal Atoms on Surfaces and Interfaces (MASI) for Sustainable Future{\textquoteright} (EP/V000055/1). E.B. acknowledges a Royal Society Wolfson Fellowship for financial support.",

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doi = "10.1021/acs.nanolett.3c01968",

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Popov, I, Ghaderzadeh, S, Kohlrausch, EC, Norman, LT, Slater, TJA, Aliev, GN, Alhabeadi, H, Kaplan, A , Theis, W, Khlobystov, AN, Fernandes, JA & Besley, E 2023, 'Chemical Kinetics of Metal Single Atom and Nanocluster Formation on Surfaces: An Example of Pt on Hexagonal Boron Nitride', Nano Letters, vol. 23, no. 17, pp. 8006-8012. https://doi.org/10.1021/acs.nanolett.3c01968

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T1 - Chemical Kinetics of Metal Single Atom and Nanocluster Formation on Surfaces

T2 - An Example of Pt on Hexagonal Boron Nitride

AU - Popov, Ilya

AU - Ghaderzadeh, Sadegh

AU - Kohlrausch, Emerson C.

AU - Norman, Luke T.

AU - Slater, Thomas J. A.

AU - Aliev, Gazi N.

AU - Alhabeadi, Hanan

AU - Kaplan, Andre

AU - Theis, Wolfgang

AU - Khlobystov, Andrei N.

AU - Fernandes, Jesum Alves

AU - Besley, Elena

N1 - Acknowledgments: This work was funded by the Engineering and Physical Sciences Research Council (EPSRC) Programme Grant ‘Metal Atoms on Surfaces and Interfaces (MASI) for Sustainable Future’ (EP/V000055/1). E.B. acknowledges a Royal Society Wolfson Fellowship for financial support.

PY - 2023/9/13

Y1 - 2023/9/13

N2 - 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.

AB - 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.

KW - single atom catalysts

KW - point defects in 2D materials

KW - nucleation kinetics

KW - metal nanoclusters

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DO - 10.1021/acs.nanolett.3c01968

M3 - Letter

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VL - 23

SP - 8006

EP - 8012

JO - Nano Letters

JF - Nano Letters

IS - 17

ER -

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

Abstract

Bibliographical note

Keywords

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Metal Atoms on Surfaces & Interfaces (MASI) for Sustainable Future

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