Atomically Dispersed Dual Metal Sites Boost the Efficiency of Olefins Epoxidation in Tandem with CO2 Cycloaddition

Tandem catalysis provides an economical and energy-efficient process for the production of fine chemicals. In this work, we demonstrate that a rationally synthesized carbon-based catalyst with atomically dispersed dual Fe-Al sites (ADD-Fe-Al) achieves superior catalytic activity for the one-pot oxidative carboxylation of olefins (conversion similar to 97%, selectivity similar to 91%), where the yield of target product over ADD-Fe-Al is at least 62% higher than that of monometallic counterparts. The kinetic results reveal that the excellent catalytic performance arises from the synergistic effect between Fe (oxidation site) and Al sites (cycloaddition site), where the efficient CO2 cycloaddition with epoxides in the presence of Al sites (3.91 wt %) positively shifts the oxidation equilibrium to olefin epoxidation over Fe sites (0.89 wt %). This work not only offers an advanced catalyst for oxidative carboxylation of olefins but also opens up an avenue for the rational design of multifunctional catalysts for tandem catalytic reactions in the future.

Automated summary

This work demonstrates that a rationally synthesized carbon-based catalyst achieves superior catalytic activity for the oxidative carboxylation of olefins. The synergistic effect between Fe and Al sites contributes to the excellent catalytic performance, providing insights for the future design of multifunctional catalysts.