CO2-generated amorphous metal organic frameworks for efficient CO2 conversion†
*ab
Abstract
Developing a feasible method to capture and utilize post-combustion CO2 in order to mitigate the adverse effects of excessive CO2 emission is a challenging task. Herein, we demonstrate a series of newly fabricated CO2-based metal–organic frameworks (MOFs) for CO2 solidification and utilization. The CO2 molecules react with deprotonated piperazine ligands, self-assemble with metal ions (Cu2+, Co2+) and generate a batch of MOFs with adjustable crystallinity from crystalline to amorphous. The crystalline MOFs can be precisely controlled by adjusting the ratio of metal sites, organic ligands and additional modulators through a bottom-up synthesis method. It is found that the amorphous CO2-based MOFs show outstanding catalytic performance for CO2 cycloaddition with epoxides (yield >99%, TOF = 218 h−1) superior to that of the corresponding crystalline ones, which is attributed to the abundant catalytic sites and accessible hierarchical pores of amorphous MOFs.
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