The development of porous MOFs exhibiting highly selective C_(2)H_(2)/CH_(4)and CO_(2)/CH_(4)separations is quite important to meet the requirement of high-purity C_(2)H_(2)and CH_(4)in various industries.By employing...The development of porous MOFs exhibiting highly selective C_(2)H_(2)/CH_(4)and CO_(2)/CH_(4)separations is quite important to meet the requirement of high-purity C_(2)H_(2)and CH_(4)in various industries.By employing a ligand heterobifunctionalization strategy,we designed and synthesized an aminopyridine-functionalized diisophthalate ligand,and successfully targeted its corresponding copper-based NbO-type MOF ZJNU-98.Gas adsorption studies revealed that ZJNU-98 exhibited significantly enhanced adsorption of C_(2)H_(2)and CO_(2)over CH_(4)compared to its parent MOF,NOTT-101.At 298 K and 1 atm,C_(2)H_(2)and CO_(2)uptakes of ZJNU-98 are 10.0%and 16.7%higher than the corresponding values of NOTT-101,while 14.2%and 18.8%increases in C_(2)H_(2)/CH_(4)and CO_(2)/CH_(4)adsorption selectivities were observed for the equimolar gas mixtures in ZJNU-98 compared to NOTT-101.Furthermore,the contribution of the functional group effect on gas adsorption has been assessed,demonstrating that the amine group plays a more important role than the pyridinic-N atom despite its lower Lewis basicity.This work provided an effective way and significant experimental evidence for the design of new porous MOFs with highly enhanced gas adsorption performance.展开更多
基金the Natural Science Foundation of China(No.21771162)the Natural Science Foundation of Zhejiang Province,China(LR16B010001)for financial support.
文摘The development of porous MOFs exhibiting highly selective C_(2)H_(2)/CH_(4)and CO_(2)/CH_(4)separations is quite important to meet the requirement of high-purity C_(2)H_(2)and CH_(4)in various industries.By employing a ligand heterobifunctionalization strategy,we designed and synthesized an aminopyridine-functionalized diisophthalate ligand,and successfully targeted its corresponding copper-based NbO-type MOF ZJNU-98.Gas adsorption studies revealed that ZJNU-98 exhibited significantly enhanced adsorption of C_(2)H_(2)and CO_(2)over CH_(4)compared to its parent MOF,NOTT-101.At 298 K and 1 atm,C_(2)H_(2)and CO_(2)uptakes of ZJNU-98 are 10.0%and 16.7%higher than the corresponding values of NOTT-101,while 14.2%and 18.8%increases in C_(2)H_(2)/CH_(4)and CO_(2)/CH_(4)adsorption selectivities were observed for the equimolar gas mixtures in ZJNU-98 compared to NOTT-101.Furthermore,the contribution of the functional group effect on gas adsorption has been assessed,demonstrating that the amine group plays a more important role than the pyridinic-N atom despite its lower Lewis basicity.This work provided an effective way and significant experimental evidence for the design of new porous MOFs with highly enhanced gas adsorption performance.
