The influences of additives of NH_3,HCl,KOH and CH_3OH on the solvothermal synthesis of the Zn-based metal-organic frameworks(Zn-MOF_5s)were investigated.Powder X-ray diffraction(PXRD),thermal gravimetric analysis(TGA...The influences of additives of NH_3,HCl,KOH and CH_3OH on the solvothermal synthesis of the Zn-based metal-organic frameworks(Zn-MOF_5s)were investigated.Powder X-ray diffraction(PXRD),thermal gravimetric analysis(TGA),Fourier translation infrared spectroscope(FT-IR),N_2adsorption/desorption at 77 K and CO_2sorption measurements were used to characterize the as-prepared Zn-MOF_5s.The experimental results showthat additives of NH_3,CH_3OH,HCl and KOH in the synthesis of the Zn-MOF_5s do not change the underlying topology,but they are extremely sensitive to the pore textural properties,thus changing the CO_2adsorption capacity.Additives would lower the pore width and the surface area,and then lower the CO_2adsorption capacity of Zn-MOF_5s.展开更多
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
A rare doubly-interpenetrating Zn-MOF(complex 1),formulated as{Zn(tci)-(bpy)(NO3)·DMF·0.5CH3CN}n(H3tci=tri(2-carboxyethyl)isocyanurate,bpy=4,4-bipyridine),has been constructed under solvothermal conditions a...A rare doubly-interpenetrating Zn-MOF(complex 1),formulated as{Zn(tci)-(bpy)(NO3)·DMF·0.5CH3CN}n(H3tci=tri(2-carboxyethyl)isocyanurate,bpy=4,4-bipyridine),has been constructed under solvothermal conditions and characterized by single-crystal X-ray diffraction,infrared spectroscopy(IR)and powder X-ray diffraction(PXRD).1 crystallizes in monoclinic system,space group C2/c with a=21.5759(4),b=12.87221(18),c=26.4917(5)Å,β=109.462(2)°,V=6937.1(2)Å3,C50H56N14O27Zn4,Mr=1546.56,Z=4,Dc=1.481 g·cm-3,μ=2.325 mm-1λ=1.54178Å,F(000)=3160,S=1.041,R=0.0621 and wR=0.1773.1 features a two-fold interpenetrating 3D hms topology.Moreover,the thermal stabilities,fluorescent and CO2 adsorption properties were investigated.Complex 1 showed highly encoura-ging photocatalytic degradation of toxic dye molecules with a potential application in wastewater purification.展开更多
基金Fujian Province Natural Science Foundation of China(No.2017J01673)
文摘The influences of additives of NH_3,HCl,KOH and CH_3OH on the solvothermal synthesis of the Zn-based metal-organic frameworks(Zn-MOF_5s)were investigated.Powder X-ray diffraction(PXRD),thermal gravimetric analysis(TGA),Fourier translation infrared spectroscope(FT-IR),N_2adsorption/desorption at 77 K and CO_2sorption measurements were used to characterize the as-prepared Zn-MOF_5s.The experimental results showthat additives of NH_3,CH_3OH,HCl and KOH in the synthesis of the Zn-MOF_5s do not change the underlying topology,but they are extremely sensitive to the pore textural properties,thus changing the CO_2adsorption capacity.Additives would lower the pore width and the surface area,and then lower the CO_2adsorption capacity of Zn-MOF_5s.
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.
基金supported by the National Natural Science Foundation of China(Nos.21401096 and 21701021)。
文摘A rare doubly-interpenetrating Zn-MOF(complex 1),formulated as{Zn(tci)-(bpy)(NO3)·DMF·0.5CH3CN}n(H3tci=tri(2-carboxyethyl)isocyanurate,bpy=4,4-bipyridine),has been constructed under solvothermal conditions and characterized by single-crystal X-ray diffraction,infrared spectroscopy(IR)and powder X-ray diffraction(PXRD).1 crystallizes in monoclinic system,space group C2/c with a=21.5759(4),b=12.87221(18),c=26.4917(5)Å,β=109.462(2)°,V=6937.1(2)Å3,C50H56N14O27Zn4,Mr=1546.56,Z=4,Dc=1.481 g·cm-3,μ=2.325 mm-1λ=1.54178Å,F(000)=3160,S=1.041,R=0.0621 and wR=0.1773.1 features a two-fold interpenetrating 3D hms topology.Moreover,the thermal stabilities,fluorescent and CO2 adsorption properties were investigated.Complex 1 showed highly encoura-ging photocatalytic degradation of toxic dye molecules with a potential application in wastewater purification.