A novel Zn-based metal–organic framework Zn(dobdc)(datz)[Zn_(2)(H2dobdc)(datz)2$1.5DMF]with plentiful hydrogen bond donors(HBD)groups was facilely synthesized from mixed ligands.The dual activation of metal Zn sites ...A novel Zn-based metal–organic framework Zn(dobdc)(datz)[Zn_(2)(H2dobdc)(datz)2$1.5DMF]with plentiful hydrogen bond donors(HBD)groups was facilely synthesized from mixed ligands.The dual activation of metal Zn sites and HBD groups for epoxides by forming Zn–O adduct and hydrogen bonds facilitated the ring-opening of epoxide substrate,which is critical for the subsequent CO_(2) fixation.Also,the existence of micropores and N-rich units in Zn(dobdc)(datz)afforded affinity towards CO_(2),which is beneficial to further improvement on catalytic CO_(2) conversion performance.Satisfactorily,Zn(dobdc)(datz)/Bu4NBr system was proved efficient heterogeneous catalyst for the CO_(2) cycloaddition with epoxides,and 98%propylene carbonate yield was obtained under mild conditions(80C,1.5 MPa and solvent-free).In addition,Zn(dobdc)(datz)/Bu4NBr exhibited remarkable versatility to different epoxides and could be completely recycled over six runs with high catalytic activity.The highly stable,easily recycle and solvent-free Zn-based MOF reported here displays eco-friendly and efficient performance to CO_(2)conversion.展开更多
基金the National Natural Science Foundation of China(21972034,21673060)the State Key Lab of Urban Water Resource and Environment of Harbin Institute of Technology(HIT2019DX12).
文摘A novel Zn-based metal–organic framework Zn(dobdc)(datz)[Zn_(2)(H2dobdc)(datz)2$1.5DMF]with plentiful hydrogen bond donors(HBD)groups was facilely synthesized from mixed ligands.The dual activation of metal Zn sites and HBD groups for epoxides by forming Zn–O adduct and hydrogen bonds facilitated the ring-opening of epoxide substrate,which is critical for the subsequent CO_(2) fixation.Also,the existence of micropores and N-rich units in Zn(dobdc)(datz)afforded affinity towards CO_(2),which is beneficial to further improvement on catalytic CO_(2) conversion performance.Satisfactorily,Zn(dobdc)(datz)/Bu4NBr system was proved efficient heterogeneous catalyst for the CO_(2) cycloaddition with epoxides,and 98%propylene carbonate yield was obtained under mild conditions(80C,1.5 MPa and solvent-free).In addition,Zn(dobdc)(datz)/Bu4NBr exhibited remarkable versatility to different epoxides and could be completely recycled over six runs with high catalytic activity.The highly stable,easily recycle and solvent-free Zn-based MOF reported here displays eco-friendly and efficient performance to CO_(2)conversion.
