Author:
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Lin, Ronghe; Albani, Davide; Fako, Edvin; Kaiser, Selina K.; Safonova, Olga V.; López, Núria; Pérez-Ramírez, Javier
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Abstract:
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Single-atom heterogeneous catalysts with welldefined
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 substratedependent
catalytic responses; structure insensitive for alkynols
with g-OH and unfunctionalized alkynes, and sensitive for
alkynols with a-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. |