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h-BN/Metal-Oxide Interface Grown by Intercalation: A Model System for Nano-Confined Catalysis


Diulus, J Trey; Novotny, Zbynek; Dongfang, Nanchen; Beckord, Jan; Al-Hamdani, Yasmine; Comini, Nicoló; Muntwiler, Matthias; Hengsberger, Matthias; Iannuzzi, Marcella; Osterwalder, Jürg (2024). h-BN/Metal-Oxide Interface Grown by Intercalation: A Model System for Nano-Confined Catalysis. Journal of Physical Chemistry C, 128(12):5156-5167.

Abstract

Deposition of two-dimensional (2D) materials onto catalyst surfaces is known to alter the adsorption energies of active sites due to the nanoconfinement effect. Traditionally, these 2D catalyst heterostructures were prepared by depositing a 2D material onto a pristine metallic surface. Preparing well-defined 2D monolayers, instead, on metal-oxide surfaces is challenging, although it is possible via O2 intercalation by oxidizing a metal substrate underneath. Several studies demonstrate this intercalative behavior of 2D covers, however, without the preparation of ordered structures, which are imperative for defining fundamental reaction mechanisms in confined space. We report the successful preparation and characterization of a well-defined, ultrathin cuprous oxide-like film grown between h-BN and Cu(111). The confined surface oxide adopts a “Cu2O-like” structure resembling the well-studied “44” Cu2O structure, although the oxidation temperature is surprisingly lower than its uncovered oxide counterpart and the h-BN layer remains intact following oxidation. Our experimental results, backed by theoretical simulations, outline the development of a heterostructure with an h-BN/metal-oxide interface as a model system, utilizing a preparation method likely transferable to a wide range of 2D/metal heterostructures and opening the door to new catalyst designs.

Abstract

Deposition of two-dimensional (2D) materials onto catalyst surfaces is known to alter the adsorption energies of active sites due to the nanoconfinement effect. Traditionally, these 2D catalyst heterostructures were prepared by depositing a 2D material onto a pristine metallic surface. Preparing well-defined 2D monolayers, instead, on metal-oxide surfaces is challenging, although it is possible via O2 intercalation by oxidizing a metal substrate underneath. Several studies demonstrate this intercalative behavior of 2D covers, however, without the preparation of ordered structures, which are imperative for defining fundamental reaction mechanisms in confined space. We report the successful preparation and characterization of a well-defined, ultrathin cuprous oxide-like film grown between h-BN and Cu(111). The confined surface oxide adopts a “Cu2O-like” structure resembling the well-studied “44” Cu2O structure, although the oxidation temperature is surprisingly lower than its uncovered oxide counterpart and the h-BN layer remains intact following oxidation. Our experimental results, backed by theoretical simulations, outline the development of a heterostructure with an h-BN/metal-oxide interface as a model system, utilizing a preparation method likely transferable to a wide range of 2D/metal heterostructures and opening the door to new catalyst designs.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Physics Institute
07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:530 Physics
Scopus Subject Areas:Physical Sciences > Electronic, Optical and Magnetic Materials
Physical Sciences > General Energy
Physical Sciences > Physical and Theoretical Chemistry
Physical Sciences > Surfaces, Coatings and Films
Language:English
Date:28 March 2024
Deposited On:23 May 2024 10:17
Last Modified:30 Jun 2024 01:41
Publisher:American Chemical Society (ACS)
ISSN:1932-7447
OA Status:Green
Publisher DOI:https://doi.org/10.1021/acs.jpcc.3c07828
Project Information:
  • : FunderH2020
  • : Grant ID801459
  • : Project TitleFP-RESOMUS - Fellowship Program of the NCCR MUST (National Competence Center for Research in Molecular Ultrafast Science and Technology) and the Cluster of Excellence RESOLV
  • : FunderSNSF
  • : Grant ID183615
  • : Project TitleNCCR MUST: Molecular Ultrafast Science and Technology (phase III)
  • : FunderSNSF
  • : Grant ID
  • : Project Title
  • Content: Submitted Version
  • Language: English
  • Description: This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in The Journal of Physical Chemistry C [Copyright © 2024 American Chemical Society] after peer review.
  • Publisher License