Acetylene (C_(2)H_(2)) and ethylene (C_(2)H_(4)) both are important chemical raw materials and energy fuel gasses.But the effective removement of trace C_(2)H_(2)from C_(2)H_(4)and the purification of C_(2)H_(2)from c...Acetylene (C_(2)H_(2)) and ethylene (C_(2)H_(4)) both are important chemical raw materials and energy fuel gasses.But the effective removement of trace C_(2)H_(2)from C_(2)H_(4)and the purification of C_(2)H_(2)from carbon dioxide(CO_(2)) are particularly challenging in the petrochemical industry.As a class of porous physical adsorbent,metal-organic frameworks (MOFs) have exhibited great success in separation and purification of light hydrocarbon gas.Herein,we rationally designed four novel MOFs by the strategy of pore space partition(PSP) via introducing triangular tri(pyridin-4-yl)-amine (TPA) into the 1D hexagonal channels of acs-type parent skeleton.By modulating the functional groups of linear dicarboxylate linkers for the parent skeleton,a series of isoreticular PSP-MOFs (SNNU-278-281) were successfully obtained.The synergistic effects of suitable pore size and Lewis basic functional groups make these MOFs ideal C_(2)H_(2)adsorbents.The gas adsorption experimental results show that all MOFs have excellent C_(2)H_(2)uptakes.Specially,SNNU-278demonstrates a high C_(2)H_(2)uptake of 149.7 cm3/g at 273 K and 1 atm.Meanwhile,SNNU-278-281 MOFs also show extremely great C_(2)H_(2)separation from CO_(2)and C_(2)H_(4).The optimized SNNU-281 with highdensity hydroxy groups exhibits extraordinary C_(2)H_(2)/CO_(2)and C_(2)H_(2)/C_(2)H_(4)dynamic breakthrough interval times up to 31 min/g and 17 min/g under 298 K and 1 bar.展开更多
基金financially supported by the National Natural Science Foundation of China (No. 22071140)the Natural Science Foundation of Shaanxi Province (No. 2021JLM-20)the Fundamental Research Funds for the Central Universities (No. GK202101002)。
文摘Acetylene (C_(2)H_(2)) and ethylene (C_(2)H_(4)) both are important chemical raw materials and energy fuel gasses.But the effective removement of trace C_(2)H_(2)from C_(2)H_(4)and the purification of C_(2)H_(2)from carbon dioxide(CO_(2)) are particularly challenging in the petrochemical industry.As a class of porous physical adsorbent,metal-organic frameworks (MOFs) have exhibited great success in separation and purification of light hydrocarbon gas.Herein,we rationally designed four novel MOFs by the strategy of pore space partition(PSP) via introducing triangular tri(pyridin-4-yl)-amine (TPA) into the 1D hexagonal channels of acs-type parent skeleton.By modulating the functional groups of linear dicarboxylate linkers for the parent skeleton,a series of isoreticular PSP-MOFs (SNNU-278-281) were successfully obtained.The synergistic effects of suitable pore size and Lewis basic functional groups make these MOFs ideal C_(2)H_(2)adsorbents.The gas adsorption experimental results show that all MOFs have excellent C_(2)H_(2)uptakes.Specially,SNNU-278demonstrates a high C_(2)H_(2)uptake of 149.7 cm3/g at 273 K and 1 atm.Meanwhile,SNNU-278-281 MOFs also show extremely great C_(2)H_(2)separation from CO_(2)and C_(2)H_(4).The optimized SNNU-281 with highdensity hydroxy groups exhibits extraordinary C_(2)H_(2)/CO_(2)and C_(2)H_(2)/C_(2)H_(4)dynamic breakthrough interval times up to 31 min/g and 17 min/g under 298 K and 1 bar.
基金supported by the National Natural Science Foundation of China (22071246 and 22272178)CAS youth interdisciplinary team (JCTD-2022-12)+1 种基金CAS-Iranian Vice presidency for science and technology joint research project (121835KYSB20200034)China Postdoctoral Science Foundation (2023M733499)。
