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      Direct Visualization of Au Atoms Bound to TiO 2(110) O-Vacancies

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          Abstract

          Au nanoparticles supported on reducible metal oxide surfaces are known to be active catalysts for a number of reactions including CO oxidation and hydrogen production. The exact choice of a metal oxide support has been shown to have a marked impact on activity, suggesting that interactions between Au and the support play a key role in catalysis. For TiO 2, a model substrate for Au catalysis, it had been thought that bridging oxygen vacancies are involved in binding Au atoms to the (110) surface based on indirect evidence. However, a recent scanning transmission electron microscopy study of single Pt atoms on TiO 2(110) suggests that subsurface vacancies are more important. To clarify the role of bridging or subsurface vacancies we employ scanning tunneling microscopy to determine the bonding site of single Au atoms on TiO 2(110). Using in situ deposition as well as a manipulation method, we provide definitive evidence that the bonding site is atop surface oxygen vacancies.

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          Onset of catalytic activity of gold clusters on titania with the appearance of nonmetallic properties

          Valden, Lai, Goodman (1998)
          Gold clusters ranging in diameter from 1 to 6 nanometers have been prepared on single crystalline surfaces of titania in ultrahigh vacuum to investigate the unusual size dependence of the low-temperature catalytic oxidation of carbon monoxide. Scanning tunneling microscopy/spectroscopy (STM/STS) and elevated pressure reaction kinetics measurements show that the structure sensitivity of this reaction on gold clusters supported on titania is related to a quantum size effect with respect to the thickness of the gold islands; islands with two layers of gold are most effective for catalyzing the oxidation of carbon monoxide. These results suggest that supported clusters, in general, may have unusual catalytic properties as one dimension of the cluster becomes smaller than three atomic spacings.
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            Identification of single-site gold catalysis in acetylene hydrochlorination.

            Adam Thetford, Li Lu, Simon Dawson … (2017)
            There remains considerable debate over the active form of gold under operating conditions of a recently validated gold catalyst for acetylene hydrochlorination. We have performed an in situ x-ray absorption fine structure study of gold/carbon (Au/C) catalysts under acetylene hydrochlorination reaction conditions and show that highly active catalysts comprise single-site cationic Au entities whose activity correlates with the ratio of Au(I):Au(III) present. We demonstrate that these Au/C catalysts are supported analogs of single-site homogeneous Au catalysts and propose a mechanism, supported by computational modeling, based on a redox couple of Au(I)-Au(III) species.
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              Enhanced bonding of gold nanoparticles on oxidized TiO2(110).

              E Laegsgaard, B. Hammer, F Besenbacher … (2007)
              We studied the nucleation of gold clusters on TiO2(110) surfaces in three different oxidation states by high-resolution scanning tunneling microscopy. The three TiO2(110) supports chosen were (i) reduced (having bridging oxygen vacancies), (ii) hydrated (having bridging hydroxyl groups), and (iii) oxidized (having oxygen adatoms). At room temperature, gold nanoclusters nucleate homogeneously on the terraces of the reduced and oxidized supports, whereas on the hydrated TiO2(110) surface, clusters form preferentially at the step edges. From interplay with density functional theory calculations, we identified two different gold-TiO2(110) adhesion mechanisms for the reduced and oxidized supports. The adhesion of gold clusters is strongest on the oxidized support, and the implications of this finding for catalytic applications are discussed.
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                Author and article information

                Journal
                Journal ID (nlm-ta): J Phys Chem C Nanomater Interfaces
                Journal ID (iso-abbrev): J Phys Chem C Nanomater Interfaces
                Journal ID (publisher-id): jy
                Journal ID (coden): jpccck
                Title: The Journal of Physical Chemistry. C, Nanomaterials and Interfaces
                Publisher: American Chemical Society
                ISSN (Print): 1932-7447
                ISSN (Electronic): 1932-7455
                Publication date (Electronic): 18 October 2017
                Publication date (Print): 09 November 2017
                Volume: 121
                Issue: 44
                Pages: 24721-24725
                Affiliations
                [† ]Department of Chemistry and London Centre for Nanotechnology, University College London , 20 Gordon Street, London WC1H 0AJ, United Kingdom
                [‡ ]Fundamental Catalysis, SABIC-CRI at KAUST , Thuwal, Saudi Arabia
                Author notes
                Article
                DOI: 10.1021/acs.jpcc.7b09608
                PMC ID: 5682598
                SO-VID: 082d0b28-f157-4cb4-89d4-e6aeb177bc81
                Copyright © Copyright © 2017 American Chemical Society
                License:

                This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.

                History
                Date received : 27 September 2017
                Date revision received : 17 October 2017
                Categories
                Subject: Article
                Custom metadata
                document-id-old-9 jp7b09608
                document-id-new-14 jp-2017-096084
                ccc-price

                ScienceOpen disciplines: Thin films & surfaces
                Data availability:
                ScienceOpen disciplines: Thin films & surfaces

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