[Chem] 我室傅钢教授和郑南峰教授发表论文:Thiol Treatment Creates Selective Palladium Catalysts for Semihydrogenation of Internal Alkynes

我室傅钢教授和郑南峰教授在 Chem 上发表论文:Thiol Treatment Creates Selective Palladium Catalysts for Semihydrogenation of Internal Alkynes

文章链接:https://www.sciencedirect.com/science/article/pii/S245192941830072X#!

摘要:

Surface and interfacial engineering of heterogeneous metal catalysts is effective and critical for optimizing selective hydrogenation for fine chemicals. By using thiol-treated ultrathin Pdnanosheets as a model catalyst, we demonstrate the development of stable, efficient, and selective Pd catalysts for semihydrogenation of internal alkynes. In the hydrogenation of 1-phenyl-1-propyne, the thiol-treated Pd nanosheets exhibited excellent catalytic selectivity (>97%) toward the semihydrogenation product (1-phenyl-1-propene). The catalyst was highly stable and showed no obvious decay in either activity or selectivity for over ten cycles. Systematic studies demonstrated that a unique Pd-sulfide/thiolate interface created by the thiol treatment was crucial to the semihydrogenation. The high catalytic selectivity and activity benefited from the combined steric and electronic effects that inhibited the deeper hydrogenation of C=C bonds. More importantly, this thiol treatment strategy is applicable to creating highly active and selective practical catalysts from commercial Pd/C catalysts for semihydrogenation of internal alkynes.