Rational Design of Alloy Catalysts for Alkyne Semihydrogenation via Descriptor-Based High-Throughput Screening

Abstract

Although alloying is a common approach to developing catalysts for alkyne selective hydrogenation, the geometric and electronic effects of active sites on the kinetics of alkyne selective hydrogenation are still ambiguous, hindering rational design of alloy catalysts. Herein, we construct structural descriptors to categorize and reorganize the roles of electronic and geometric factors in the kinetics of acetylene semihydrogenation. The prediction model based on our proposed structural descriptors successfully elucidates the activity and selectivity trends among Pd-based alloys and can also be extended to rationalize the kinetics trend among single-atom alloys and Ni-based alloys for semihydrogenation of acetylene and even other alkynes, in good agreement with available experimental references. Aided by thermodynamic stability analysis and structural descriptors, 489 Pd-based bimetallic alloys via a high-throughput screening protocol were evaluated, and finally, Pd 1 Nb 3 and Pd 1 Hf 3 were identified with a high yield of ethylene and inexpensive cost and validated by our experimental studies.