Facile prepared 2D Ni-based metal-organic framework nanosheets for boosting one-pot catalytic synthesis of cyclic carbonates

Two isostructural Ni-based MOF 2D nanosheets (NiBDC NS and NiBDC-NH2 NS) were facilely constructed by reflux method, which exhibited excellent activity for one-pot epoxidation-CO2 cycloaddition catalysis. Combining our activity evaluations, detailed kinetics and molecular simulation results, we revealed that the amino groups of these materials played a positive role in CO2 cycloaddition step but a negative role in epoxidation step. By using NiBDC NS, the conversion and yield of the targeted products under mild condition (80 °C, 1 bar and 12 h) could achieve 95% and 87%, respectively. The calculated Thiele modulus and effectiveness factor indicated that NiBDC NS exhibited a higher catalyst utilization degree with negligible diffusion constraint. We further confirmed the stability of these catalysts by repeatedly running the catalysis six times without observing significant loss of activity. Finally, the reaction mechanism was proposed by combining the results from experiment and simulations.