Encapsulation of Palladium Carbide Subnanometric Species in Zeolite Boosts Highly Selective Semihydrogenation of Alkynes

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Abstract
The selective hydrogenation of alkynes to alkenes is a crucial step in the synthesis of fine chemicals. However, the widely utilized palladium (Pd)‐based catalysts often suffer from poor selectivity. In this work, we demonstrate a carbonization‐reduction method to create palladium carbide subnanometric species within pure silicate MFI zeolite. The carbon species can modify the electronic and steric characteristics of Pd species by forming the predominant Pd−C4 structure and, meanwhile, facilitate the desorption of alkenes by forming the Si−O−C structure with zeolite framework, as validated by the state‐of‐the‐art characterizations and theoretical calculations. The developed catalyst shows superior performance in the selective hydrogenation of alkynes over mild conditions (298 K, 2 bar H2), with 99 % selectivity to styrene at a complete conversion of phenylacetylene. In contrast, the zeolite‐encapsulated carbon‐free Pd catalyst and the commercial Lindlar catalyst show only 15 % and 14 % selectivity to styrene, respectively, under identical reaction conditions. The zeolite‐confined Pd‐carbide subnanoclusters promise their superior properties in semihydrogenation of alkynes.
Funding Information
  • ShanghaiTech University (EM02161943)
  • National Natural Science Foundation of China (21920102005, 22288101, 21835002, 22201094, 91961119)
  • National Key Research and Development Program of China (2021YFA1501202)
  • Higher Education Discipline Innovation Project (B17020)
  • Fundación Carmen y Severo Ochoa (SEV-2016-0683)

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