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Maximizing the Number of Interfacial Sites in Single‐Atom Catalysts for the Highly Selective, Solvent‐Free Oxidation of Primary Alcohols
Author(s) -
Li Tianbo,
Liu Fei,
Tang Yan,
Li Lin,
Miao Shu,
Su Yang,
Zhang Junying,
Huang Jiahui,
Sun Hui,
Haruta Masatake,
Wang Aiqin,
Qiao Botao,
Li Jun,
Zhang Tao
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.201803272
Subject(s) - oxidizing agent , catalysis , selectivity , alcohol oxidation , solvent , metal , chemistry , alcohol , oxide , atom (system on chip) , nanoparticle , substrate (aquarium) , heterogeneous catalysis , photochemistry , inorganic chemistry , combinatorial chemistry , materials science , organic chemistry , nanotechnology , oceanography , geology , computer science , embedded system
The solvent‐free selective oxidation of alcohols to aldehydes with molecular oxygen is highly attractive yet challenging. Interfacial sites between a metal and an oxide support are crucial in determining the activity and selectivity of such heterogeneous catalysts. Herein, we demonstrate that the use of supported single‐atom catalysts (SACs) leads to high activity and selectivity in this reaction. The significantly increased number of interfacial sites, resulting from the presence of individually dispersed metal atoms on the support, renders SACs one or two orders of magnitude more active than the corresponding nanoparticle (NP) catalysts. Lattice oxygen atoms activated at interfacial sites were found to be more selective than O 2 activated on metal NPs in oxidizing the alcohol substrate. This work demonstrates for the first time that the number of interfacial sites is maximized in SACs, providing a new avenue for improving catalytic performance by developing appropriate SACs for alcohol oxidation and other reactions occurring at metal–support interfacial sites.