Linear-Structure Single-Atom Gold(I) Catalyst for Dehydrogenative Coupling of Organosilanes with Alcohols Article Swipe
Ravishankar G. Kadam
,
Miroslav Medveď
,
Subodh Kumar
,
Dagmar Zaoralová
,
Giorgio Zoppellaro
,
Zdeňěk Baďura
,
Tiziano Montini
,
Aristides Bakandritsos
,
Emiliano Fonda
,
Ondřej Tomanec
,
Michal Otyepka
,
Rajender S. Varma
,
Manoj B. Gawande
,
Paolo Fornasiero
,
Radek Zbořil
·
YOU?
·
· 2023
· Open Access
·
· DOI: https://doi.org/10.1021/acscatal.3c03937
YOU?
·
· 2023
· Open Access
·
· DOI: https://doi.org/10.1021/acscatal.3c03937
A strategy for the synthesis of a gold-based single-atom catalyst (SAC) via a one-step room temperature reduction of Au(III) salt and stabilization of Au(I) ions on nitrile-functionalized graphene (cyanographene; G-CN) is described. The graphene-supported G(CN)-Au catalyst exhibits a unique linear structure of the Au(I) active sites promoting a multistep mode of action in dehydrogenative coupling of organosilanes with alcohols under mild reaction conditions as proven by advanced XPS, XAFS, XANES, and EPR techniques along with DFT calculations. The linear structure being perfectly accessible toward the reactant molecules and the cyanographene-induced charge transfer resulting in the exclusive Au(I) valence state contribute to the superior efficiency of the emerging two-dimensional SAC. The developed G(CN)-Au SAC, despite its low metal loading (ca. 0.6 wt %), appear to be the most efficient catalyst for Si-H bond activation with a turnover frequency of up to 139,494 h-1 and high selectivities, significantly overcoming all reported homogeneous gold catalysts. Moreover, it can be easily prepared in a multigram batch scale, is recyclable, and works well toward more than 40 organosilanes. This work opens the door for applications of SACs with a linear structure of the active site for advanced catalytic applications.
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Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acscatal.3c03937
- OA Status
- hybrid
- Cited By
- 13
- References
- 50
- Related Works
- 10
- OpenAlex ID
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All OpenAlex metadata
Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4389173922Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1021/acscatal.3c03937Digital Object Identifier
- Title
-
Linear-Structure Single-Atom Gold(I) Catalyst for Dehydrogenative Coupling of Organosilanes with AlcoholsWork title
- Type
-
articleOpenAlex work type
- Language
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enPrimary language
- Publication year
-
2023Year of publication
- Publication date
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2023-11-30Full publication date if available
- Authors
-
Ravishankar G. Kadam, Miroslav Medveď, Subodh Kumar, Dagmar Zaoralová, Giorgio Zoppellaro, Zdeňěk Baďura, Tiziano Montini, Aristides Bakandritsos, Emiliano Fonda, Ondřej Tomanec, Michal Otyepka, Rajender S. Varma, Manoj B. Gawande, Paolo Fornasiero, Radek ZbořilList of authors in order
- Landing page
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https://doi.org/10.1021/acscatal.3c03937Publisher landing page
- Open access
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YesWhether a free full text is available
- OA status
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hybridOpen access status per OpenAlex
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https://doi.org/10.1021/acscatal.3c03937Direct OA link when available
- Concepts
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Catalysis, Chemistry, Graphene, Valence (chemistry), X-ray photoelectron spectroscopy, Molecule, Combinatorial chemistry, Hydrosilylation, Photochemistry, Materials science, Organic chemistry, Nanotechnology, Chemical engineering, EngineeringTop concepts (fields/topics) attached by OpenAlex
- Cited by
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13Total citation count in OpenAlex
- Citations by year (recent)
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2025: 6, 2024: 7Per-year citation counts (last 5 years)
- References (count)
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50Number of works referenced by this work
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-
10Other works algorithmically related by OpenAlex
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