Efficient separation of ethylene(C_(2)H_(4))from ethane(C_(2)H_(6))via a one-step adsorption process is desirable yet challenging.In this work,we report a C_(2)H_(6)-selective polynuclear Tb-MOF[Tb_(9)(μ_(3)-O)_(2)(...Efficient separation of ethylene(C_(2)H_(4))from ethane(C_(2)H_(6))via a one-step adsorption process is desirable yet challenging.In this work,we report a C_(2)H_(6)-selective polynuclear Tb-MOF[Tb_(9)(μ_(3)-O)_(2)(μ_(3)-OH)_(12)(H_(2)O)_(9)(TCPE)_(3)]^(−)·[H_(3)O]^(+)·(solvents)_(x)(TCPE=tetrakis(4-carboxyphenyl)ethylene acid),NKU-200-Tb,assembled via the reticular chemistry principle.The resulting(4,12)-connected framework critically features a high density of nonpolar aromatic rings on the pore surface and forms a specific nanotrap for C_(2)H_(6)with multiple C-H…π interaction sites.As a result,NKU-200-Tb exhibits an inverse adsorption behavior with a high C_(2)H_(6)/C_(2)H_(4)selectivity of 2.06 and a large uptake ratio of 151%(60.27/39.95 cm^(3)g^(−1))at 298 K and 1 bar.The superior adsorption properties of NKU-200-Tb,combined with great structural stability,place it among the most promising stable C_(2)H_(6)-selective MOFs.Dynamic breakthrough experiments demonstrate that polymer-grade C_(2)H_(4)(>99.9%)can be harvested in one step from a binary mixture of C_(2)H_(6)/C_(2)H_(4)(10/90,v/v).This work signifies the synergy of pore surface chemistry and space confinement in promoting the challenging C_(2)H_(6)/C_(2)H_(4)separation.展开更多
基金supported by the National Natural Science Foundation of China(22171144 and 22001132)the Fundamental Research Funds for the Central Universities(Nankai University).
文摘Efficient separation of ethylene(C_(2)H_(4))from ethane(C_(2)H_(6))via a one-step adsorption process is desirable yet challenging.In this work,we report a C_(2)H_(6)-selective polynuclear Tb-MOF[Tb_(9)(μ_(3)-O)_(2)(μ_(3)-OH)_(12)(H_(2)O)_(9)(TCPE)_(3)]^(−)·[H_(3)O]^(+)·(solvents)_(x)(TCPE=tetrakis(4-carboxyphenyl)ethylene acid),NKU-200-Tb,assembled via the reticular chemistry principle.The resulting(4,12)-connected framework critically features a high density of nonpolar aromatic rings on the pore surface and forms a specific nanotrap for C_(2)H_(6)with multiple C-H…π interaction sites.As a result,NKU-200-Tb exhibits an inverse adsorption behavior with a high C_(2)H_(6)/C_(2)H_(4)selectivity of 2.06 and a large uptake ratio of 151%(60.27/39.95 cm^(3)g^(−1))at 298 K and 1 bar.The superior adsorption properties of NKU-200-Tb,combined with great structural stability,place it among the most promising stable C_(2)H_(6)-selective MOFs.Dynamic breakthrough experiments demonstrate that polymer-grade C_(2)H_(4)(>99.9%)can be harvested in one step from a binary mixture of C_(2)H_(6)/C_(2)H_(4)(10/90,v/v).This work signifies the synergy of pore surface chemistry and space confinement in promoting the challenging C_(2)H_(6)/C_(2)H_(4)separation.
