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Design of Single Gold Atoms on Nitrogen‐Doped Carbon for Molecular Recognition in Alkyne Semi‐Hydrogenation
Author(s) -
Lin Ronghe,
Albani Davide,
Fako Edvin,
Kaiser Selina K.,
Safonova Olga V.,
López Núria,
PérezRamírez Javier
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201805820
Subject(s) - alkyne , substrate (aquarium) , catalysis , carbon fibers , chemistry , atom (system on chip) , combinatorial chemistry , doping , metal , nitrogen atom , nanotechnology , photochemistry , chemical physics , materials science , organic chemistry , optoelectronics , oceanography , composite number , computer science , composite material , embedded system , geology , group (periodic table)
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.