Green carboxylation of CO2 triggered by well-dispersed silver nanoparticles immobilized by melamine-based porous organic polymers

Abstract

CO2 fixation via directly formation of C-C bonds to obtain carboxylation compound is an essential reaction in industry. Creating efficient, inexpensive and industrially valuable key catalysts have always been a desire, but also an urgent challenge. Here, we synthesized a kind of melamine-based porous organic polymers (POPs) evenly loaded Ag Nanoparticles (Ag NPs/Melamine-based POPs) by the gas bubbling-assisted membrane reduction (GBMR) approach. The melamine-based POPs were used as good nitrogen-rich supports for loading and dispersing Ag nanoparticles. Ag NPs/ melamine-based POPs exhibited good CO2 absorption capacity (2.1 mmol/g, 273 K and 0.1 MPa) and the excellent activity was up to 93% towards the carboxylation of terminal alkynes with CO2 under mild reaction conditions (323 K, 0.1 MPa). And the TOF is 2.23 h−1. Specially, this is very few report of heterogeneously catalyzed directly formation of carboxylation compound only applying terminal alkynes with CO2 under low temperature and atmospheric pressure. The mechanistic study revealed that the well-dispersed Ag active species promoted highly efficient and green conversion of CO2. Moreover, the catalyst was easily recovered and could be reused at least six times with retention of high catalytic activity.