Isolated Palladium Atoms Dispersed on Silicoaluminophosphate-31 (SAPO-31) for the Semihydrogenation of Alkynes

Supported single-atom catalysts have become one of the most exciting frontiers in heterogeneous catalysis. The physicochemical properties of these materials are highly interesting; however, the generation of stable single atoms on solid supports is still challenging. Herein, we report an efficient and operationally simple postsynthesis method, consisting of spatial confining, freeze-drying, and reducing steps, for the construction of singly dispersed palladium atoms on SAPO-31 (Pd-1/SAPO-31) with promising application prospects in the semihydrogenation of alkynes. A typical Pd-N-C single-atom catalyst derived from the ZIF-8-supported palladium complex was prepared and compared to Pd-1/SAPO-31. The Pd-1/SAPO-31 catalyst showed outstanding performance in the semihydrogenation of both phenylacetylene (85% selectivity at 99% conversion, 40 min) and 1-chloro-4-ethynylbenzene (95% selectivity at 99% conversion, 60 min). In addition, this single-atom palladium catalyst was highly active in triethoxysilane oxidation. Most importantly, this catalyst retained its atomic dispersion and catalytic activity after high-temperature thermal treatment in Ar at 700 degrees C. This study demonstrates how zeolites can be used to confine atomically dispersed metal species and tune the activity and stability of these materials to meet the needs of practical applications.

Automated summary

Supported single-atom catalysts are at the forefront of heterogeneous catalysis, with physicochemical properties that are highly interesting. This study demonstrates an efficient postsynthesis method for constructing singly dispersed palladium atoms on SAPO-31, showing promising application prospects in the semihydrogenation of alkynes. The catalyst exhibited outstanding performance in the semihydrogenation of phenylacetylene and 1-chloro-4-ethynylbenzene, as well as high activity in triethoxysilane oxidation, with retention of atomic dispersion and catalytic activity at high temperatures.