Abstract
Selective chemical fixation of CO2 represents a promising approach to mitigate escalating atmospheric CO2 concentration and synthesizing essential commodity chemicals to boost the circular economy. The cycloaddition of CO2 for producing α‐alkylidene cyclic carbonates is an attractive research topic as it uses cheap CO2 as C1 feedstock in a 100% atom economy reaction. Hence, we designed an amine‐functionalized, nitrogen‐rich COF (SNW‐1@NH2) to strongly graft Cu(I) ions within its pores. The synergistic effect of both SNW‐1@NH2 and Cu(I) ion boosted the catalytic activity towards precious metal‐free CO2 cycloaddition with propargylic alcohol to produce α‐alkylidene cyclic carbonate at room temperature. Furthermore, broad substrate scope and high recyclability of the catalyst with retention of catalytic activity and structural integrity were observed. Contrarily, SNW‐1@NH2 was further employed for catalytic Knoevenagel condensation reaction between benzaldehyde and cyanoacetamide. SNW‐1@NH2 COF yielded desired products in Knoevenagel condensation with broad substrate scope and high recyclability without affecting its structural integrity and functionality. Additionally, deep mechanistic investigations were executed to describe plausible catalytic pathways for both catalysis reactions. We hope that this investigation towards developing nitrogen‐rich porous soft materials and expanding its applicability can offer alternative solutions to multiple severe environmental concerns.
Published Version
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