Highly Active and Stable Palladium Single-Atom Catalyst Achieved by a Thermal Atomization Strategy on an SBA-15 Molecular Sieve for Semi-Hydrogenation Reactions.

Single-atom catalysts (SACs) have great potential to revolutionize heterogeneous catalysis, enabling fast and direct construction of desired products. Given their notable promise, a general and scalable strategy to access these catalyst systems is highly desirable. Herein, we describe a straightforward and efficient thermal atomization strategy to create atomically dispersed palladium atoms anchored on a nitrogen-doped carbon shell over an SBA-15 support. Their presence was confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurement. The nitrogen-containing carbon shells provide atomic diffusion sites for anchoring palladium atoms emitted from palladium nanoparticles. This catalyst showed exceptional efficiency in selective hydrogenation of phenylacetylene and other types of alkynes. Importantly, it showed excellent stability, recyclability, and sintering-resistant ability. This approach can be scaled up with comparable catalytic activity. We anticipate that this work may lay the foundation for rapid access to high-quality SACs that are amenable to large-scale production for industrial applications.