Metal

Alcohol

Catalysis

Engineering

Oxide

Nanoparticle

Photochemistry

Materials science

Embedded system

Solvent

Computer science

Inorganic chemistry

Chemical engineering

Substrate (aquarium)

Geology

Oceanography

Oxidizing agent

Combinatorial chemistry

Alcohol oxidation

Nanotechnology

Organic chemistry

Atom (system on chip)

Chemistry

Selectivity

Heterogeneous catalysis

Angewandte Chemie International Edition

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.

Maximizing the Number of Interfacial Sites in Single‐Atom Catalysts for the Highly Selective, Solvent‐Free Oxidation of Primary Alcohols