• • Pd1/ZnO-1.9 nm catalyst achieves a TOF of 25.6 min-1 in acetylene semi-hydrogenation, a 25-fold increase over bulk Pd1/ZnO (1.0 min-1), directly enabling higher throughput and reduced reactor volume in industrial ethylene purification.
• • Reducing ZnO particle size from ~46 nm to ~1.9 nm shifts the LUMO from -0.35 V to -1.12 V (vs. NHE) and broadens the band gap from 3.29 eV to 5.82 eV, providing a tunable electronic descriptor for optimizing metal-support orbital coupling.
• • The Pd1/ZnO-1.9 nm catalyst maintains exceptional stability and selectivity for 100 h, outperforming Pd1/ZnO-8.5 nm and bulk counterparts, which is critical for continuous industrial operation and minimizing catalyst regeneration costs.
• • A total of 34 Pd1/MOx SACs with 0.1 wt% Pd loading were synthesized across 14 MOx compositions (ZnO, CoOx, NiOx, TiO2, Ga2O3), demonstrating the generality of the LUMO-activity correlation and enabling predictive design of SACs for diverse catalytic applications.