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[JACS] 我室郑南峰教授发表论文:Hydrogen Bond Network Induced by Surface Ligands Shifts the Semi-hydrogenation Selectivity over Palladium Catalysts

发布日期:2023年05月04日   浏览次数:

我室郑南峰教授在 JACS 上发表论文:Hydrogen Bond Network Induced by Surface Ligands Shifts the Semi-hydrogenation Selectivity over Palladium Catalysts

摘要:Tuning the metal–ligand interfaces of heterogeneous catalysts has emerged as an effective strategy to optimize their catalytic performance. However, improving the selectivity via organic modification remains a challenge so far. In this work, we demonstrate a simple ligand modification by preparing cysteamine-coated ultrathin palladium nanosheets. The as-prepared catalyst exhibits excellent selectivity with durability during catalytic hydrogenation of terminal alkynes, superior to most previously reported ligand-protected palladium catalysts. Further study reveals that a zwitterionic transformation occurs on the palladium interface under the H2 conditions, generating a rigid hydrogen bond network. Such an unexpected effect beyond the traditional steric effect derived from van der Waals interactions makes the catalytic surface favor the hydrogenation of alkynes over alkenes without significantly sacrificing the catalytic activity. These results not only provide a unique steric effect concept for surface coordination chemistry but also provide a practical application to improve the selectivity and activity comprehensively.

文章链接:https://pubs.acs.org/doi/10.1021/jacs.3c00953