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

Abstract

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 (Pd1/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 Pd1/SAPO-31. The Pd1/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 °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.