AI Article Synopsis
- Single-atom heterogeneous catalysts can improve our understanding of how architecture affects performance, but adjusting the metal's structure and properties is complex.
- A new method allows for the precise manipulation of gold atoms on N-doped carbon surfaces by varying activation temperatures and altering surrounding coordination neighbors, as well as the metal's oxidation state.
- Catalytic tests reveal that gold catalysts show different performances depending on the type of alkyne, with specific substrate interactions enhancing activity, which is explained through density functional theory linking these responses to gold-cavity ensembles.
Article Abstract
Single-atom heterogeneous catalysts with well-defined architectures are promising for deriving structure-performance relationships, but the challenge lies in finely tuning the structural and electronic properties of the metal. To tackle this point, a new approach based on the surface diffusion of gold atoms on different cavities of N-doped carbon is presented. By controlling the activation temperature, the coordination neighbors (Cl, O, N) and the oxidation state of the metal can be tailored. Semi-hydrogenation of various alkynes on the single-atom gold catalysts displays substrate-dependent catalytic responses; structure insensitive for alkynols with γ-OH and unfunctionalized alkynes, and sensitive for alkynols with α-OH. Density functional theory links the sensitivity for alkynols to the strong interaction between the substrate and specific gold-cavity ensembles, mimicking a molecular recognition pattern that allows to identify the cavity site and to enhance the catalytic activity.
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| http://dx.doi.org/10.1002/anie.201805820 | DOI Listing |
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