3 years ago

Design of Single Gold Atoms on Nitrogen‐Doped Carbon for Molecular Recognition in Alkyne Semi‐hydrogenation

Ronghe Lin, Davide Albani, Edvin Fako, Selina K Kaiser, Olga V Safonova, Núria López, Javier Pérez-Ramírez

Abstract

Single‐atom heterogeneous catalysts with well‐defined architectures are promising for deriving structure‐performance relations, but the challenge lies in finely tuning the structural and electronic properties of the metal. To tackle this point, a new approach is reported based on the differential surface diffusion of gold atoms on different cavities of N‐doped carbon. By controlling the activation temperature, the coordination neighbors (Cl, O, and 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 gamma‐OH and unfunctionalized alkynes, and sensitive for alkynols with alpha‐OH. Density functional theory links the latter phenomenon to the strong interaction between the substrate and specific gold‐cavity ensembles, mimicking a molecular recognition pattern that allows to identify the cavity structure and to enhance the catalytic performance.

Publisher URL: https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201805820

DOI: 10.1002/anie.201805820

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