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Surface Reconstruction of Ag and Au–Ag Model Nano-catalysts During Exposure to Oxidising Gas Atmospheres

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Abstract

At the industrial level, Ag catalysts in the form of silver crystals held by a silver gauze are largely used for formaldehyde production and ethylene epoxidation. These self-supported structures undergo surface reconstructions and morphological changes upon exposure to moderately high temperatures (473–900 K) and oxidising atmospheres. These phenomena have been studied and well understood on single crystal surfaces and polycrystalline foils: different oxygen surface and sub-surface species have been identified and reconstruction processes explained. To verify the scalability of the surface science results and ultimately understand these phenomena on catalysts at the industrial scale, further studies on more complex samples are needed. Attempts to close this “materials gap” have been carried out in this present study where experiments have been performed on model single catalytic nanoparticles, i.e. the apexes of field emitter tips, using both field emission (FE) and field ion (FI) microscopies. Pure Ag samples are exposed to a pressure of 3 × 10–5 mbar of O2 at temperatures up to 700 K. These conditions reflect those used on the industrial scale. Important surface/morphological reconstructions are observed both in FE and FI modes. For comparison, experiments have been repeated on Au-8.8%at. Ag field emitter tips, representative samples for Au–Ag catalytic nanofoams, using to 3 × 10–5 mbar of NO2 at temperatures up to 450 K. Similar behaviour are observed and the influence of the oxidising gas is discussed.

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Funding

Luc Jacobs and Cédric Barroo thank the Fonds de la Recherche Scientifique (F.R.S.-FNRS) for financial support: PhD grant from FRIA (L.J.) and postdoctoral fellowship from FNRS (C.B.).The authors thanks Dr. Eric Genty for fruitful discussions.

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Authors and Affiliations

  1. Chemistry of Surfaces, Interfaces and Nanomaterials (ChemSIN) – Catalysis, Université Libre de Bruxelles, CP243, Brussels, Belgium

    Luc Jacobs, Cédric Barroo & Thierry Visart de Bocarmé

  2. Center for Nonlinear Phenomena and Complex Systems (CENOLI), Université Libre de Bruxelles, CP231, Brussels, Belgium

    Cédric Barroo & Thierry Visart de Bocarmé

Authors
  1. Luc Jacobs
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  2. Cédric Barroo
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  3. Thierry Visart de Bocarmé
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Contributions

Funding of the project: L.J., C.B., T.V., Design and realisation of the experiments: L.J., C.B., Interpretation of the data: L.J., C.B., Manuscript writing: L.J., Manuscript review, L.J., C.B., T.V.

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Correspondence to Luc Jacobs.

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All authors declare that they have no conflict of interest.

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All used materials are commercially available. Precise information on the presented data are available upon request.

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Jacobs, L., Barroo, C. & Visart de Bocarmé, T. Surface Reconstruction of Ag and Au–Ag Model Nano-catalysts During Exposure to Oxidising Gas Atmospheres. Top Catal 63, 1569–1577 (2020). https://doi.org/10.1007/s11244-020-01365-1

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  • DOI: https://doi.org/10.1007/s11244-020-01365-1

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