High-Density and Thermally Stable Palladium Single-Atom Catalysts for Chemoselective Hydrogenations
Ying Ma1,2, Yujing Ren1, Yanan Zhou3,4
1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Science, 457 Zhongshan Road, Dalian, 116023, China.
Abstract:
Single-atom catalysts (SACs) have shown superior activity and/or selectivity for many energy- and environment-related reactions, but their stability at high site density and under reducing atmosphere remains unresolved. Herein, we elucidate the intrinsic driving force of a Pd single atom with high site density (up to 5 wt %) under reducing atmosphere, and its unique catalytic performance for hydrogenation reactions. In situ experiments and calculations reveal that Pd atoms tend to migrate into the surface vacancy-enriched MoC surface during the carburization process by transferring oxide crystals to carbide crystals, leading to the surface enrichment of atomic Pd instead of formation of particles. The Pd1 /α-MoC catalyst exhibits high activity and excellent selectivity for liquid-phase hydrogenation of substituted nitroaromatics (>99 %) and gas-phase hydrogenation of CO2 to CO (>98 %). The Pd1 /α-MoC catalyst could endure up to 400 °C without any observable aggregation of single atoms.
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