摘要
A new approach to allylic alkylation is realized using an atomically dispersed palladium catalyst(Pd1/TiO2-EG).Unlike conventional methods that require derivation of substrates and utilization of additives,this method allows for direct allylic alkylation from allylic alcohols,producing H2O as the sole by-product.The catalyst's high efficiency is attributed to the local hydrogen bonding at the or-ganic-inorganic interface(Pd-EG interface),facilitating hydroxyl group activation forη3π-allyl complex formation.The system demonstrates successful direct C—O and C—C coupling reactions with high selectivity,requiring no additives.This study highlights the potential of supported atomically dispersed catalysts for greener and more efficient catalysis,meanwhile,offers unique insights into the distinct behavior of atomically dispersed catalysts in comparison to homogeneous or nanoparticle-based catalysts.
基金
support from National Key R&D Program of China (2022YFA1504500)
the National Natural Science Foundation of China (grant no.92261207,and NSFC Center for Single-Atom Catalysis under grant no.22388102)
the New Cornerstone Science Foundation.P.L.acknowledges the Shanghai Pujiang Talent Program (No.21PJ1410400)
the Start-up Funding and the Double First-Class Initiative Fund of ShanghaiTech University.R.Q.acknowledges support from the Young Scientists Fund of the National Natural Science Foundation of China (22202164)
the Natural Science Foundation of Fujian Province (2023J05006)
the Fundamental Research Funds for the Central Universities (20720230002)
the Fujian Provincial Chemistry Discipline Alliance.