Single-atom catalysis represents
a new frontier that integrates
the merits of homogeneous and heterogeneous catalysis to afford exceptional
atom efficiency, activity, and selectivity for a range of catalytic
systems. Herein we describe a simple defect engineering strategy to
construct an atomically dispersed palladium catalyst (Pdδ+, 0 < δ < 2) by anchoring the palladium atoms on oxygen
vacancies created in CeO2 nanorods. This was confirmed
by spherical aberration correction electron microscopy and extended
X-ray absorption fine structure measurement. The as-prepared catalyst
showed exceptional catalytic performance in the hydrogenation of styrene
(99% conversion, TOF of 2410 h–1), cinnamaldehyde
(99% conversion, 99% selectivity, TOF of 968 h–1), as well as oxidation of triethoxysilane (99% conversion, 79 selectivity,
TOF of 10 000 h–1). This single-atom palladium
catalyst can be reused at least five times with negligible activity
decay. The palladium atoms retained their dispersion on the support
at the atomic level after thermal stability testing in Ar at 773 K.
Most importantly, this synthetic method can be scaled up while maintaining
catalytic performance. We anticipate that this method will expedite
access to single-atom catalysts with high activity and excellent resistance
to sintering, significantly impacting the performance of this class
of catalysts.