<p>Direct synthesis of high-value-added chemicals from low-carbon molecules is of great research importance. The C(sp<sup>3</sup>)—H bonds in alkanes exhibit a high bond dissociation energy and a very low polarity; consequently, achieving highly selective synthesis of esters through alkoxy carbonylation in heterogeneous catalysis is a particularly challenging process. Herein, we describe the immobilization of a single-atom palladium catalyst supported by porous organic polymers for highly selective ester formation in cycloalkane carbonylation, which achieves a selectivity as high as 82% and a benzyl alcohol conversion of up to 96%. Various catalytic characterization methods, including XRD, XPS, TEM, SEM, and FTIR, indicate that palladium species are uniformly distributed in the polymer. This work suggests a promising method for the design of hybrid catalytic systems and offers meaningful insights into the development of bifunctional catalysts for selective alkoxy carbonylation.</p>

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Porous polymer-supported palladium catalyst for highly selective catalysis of cycloalkane carbonyl esterification

  • Mingqin Guo,
  • Ce Liu,
  • Hangkong Yuan,
  • Xunxun Li,
  • Delong Han,
  • Xinjiang Cui

摘要

Direct synthesis of high-value-added chemicals from low-carbon molecules is of great research importance. The C(sp3)—H bonds in alkanes exhibit a high bond dissociation energy and a very low polarity; consequently, achieving highly selective synthesis of esters through alkoxy carbonylation in heterogeneous catalysis is a particularly challenging process. Herein, we describe the immobilization of a single-atom palladium catalyst supported by porous organic polymers for highly selective ester formation in cycloalkane carbonylation, which achieves a selectivity as high as 82% and a benzyl alcohol conversion of up to 96%. Various catalytic characterization methods, including XRD, XPS, TEM, SEM, and FTIR, indicate that palladium species are uniformly distributed in the polymer. This work suggests a promising method for the design of hybrid catalytic systems and offers meaningful insights into the development of bifunctional catalysts for selective alkoxy carbonylation.