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Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts
Author(s) -
Xin Pingyu,
Li Jia,
Xiong Yu,
Wu Xi,
Dong Juncai,
Chen Wenxing,
Wang Yu,
Gu Lin,
Luo Jun,
Rong Hongpan,
Chen Chen,
Peng Qing,
Wang Dingsheng,
Li Yadong
Publication year - 2018
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201801103
Subject(s) - catalysis , palladium , cerium , alcohol oxidation , cerium oxide , chemistry , alcohol , benzaldehyde , transmission electron microscopy , cluster (spacecraft) , metal , selectivity , oxide , inorganic chemistry , materials science , nanotechnology , organic chemistry , computer science , programming language
The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd 1 /CeO 2 ) and hexapalladium cluster–cerium oxide (Pd 6 /CeO 2 ), as confirmed by spherical‐aberration‐corrected transmission electron microscopy and X‐ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd 1 /CeO 2 shows extremely high catalytic activity with a TOF of 6739 h −1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd 6 /CeO 2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd 6 clusters hinder the interactions between hydroxy groups and the CeO 2 surface, thus suppressing synergy of Pd‐Ce perimeter.