Porous ionic liquids have demonstrated excellent performance in the field of separation,attributed to their high specific surface area and efficient mass transfer.Herein,task-specific protic porous ionic liquids(PPILs...Porous ionic liquids have demonstrated excellent performance in the field of separation,attributed to their high specific surface area and efficient mass transfer.Herein,task-specific protic porous ionic liquids(PPILs)were prepared by employing a novel one-step coupling neutralization reaction strategy for extractive desulfurization.The single-extraction efficiency of PPILs reached 75.0%for dibenzothiophene.Moreover,adding aromatic hydrocarbon interferents resulted in a slight decrease in the extraction efficiency of PPILs(from 45.2%to 37.3%,37.9%,and 33.5%),indicating the excellent extraction selectivity of PPILs.The experimental measurements and density functional theory calculations reveal that the surface channels of porous structures can selectively capture dibenzothiophene by the stronger electrophilicity(Eint(HS surface channel/DBT)=-39.8 kcal mol^(-1)),and the multiple extraction sites of ion pairs can effectively enrich and transport dibenzothiophene from the oil phase into PPILs throughπ...π,C-H...πand hydrogen bonds interactions.Furthermore,this straightforward synthetic strategy can be employed in preparing porous liquids,offering new possibilities for synthesizing PPILs with tailored functionalities.展开更多
Porous liquids,which are liquids with permanent porosity,have received significant attention as a new class of materials with the potential for far-reaching impacts in a variety of applications including gas separatio...Porous liquids,which are liquids with permanent porosity,have received significant attention as a new class of materials with the potential for far-reaching impacts in a variety of applications including gas separation.In this work,in situ Fourier transform infrared spectroscopy measurements were conducted to investigate the mechanism of carbon dioxide absorption in a porous ionic liquid consisting of ZIF-8 combined with 8,80-(3,6-dioxaoctane-1,8-diyl)bis(1,8-diazabicyclo[5.4.0]undec-7-en-8-ium)bis(trifluoromethanesulfonyl)imide([DBU-PEG][(Tf_(2)N)_(2)]).While the vibrational modes of the pure ionic liquid remain relatively unchanged,the incorporation of carbon dioxide leads to slight structural fluctuations in the ZIF-8 framework whether it is pure solid or as integrated into the porous ionic liquid.The analysis of the vibrational modes of the porous ionic liquid suggests that the interaction of the CO_(2) occurs more strongly with the ring structure of the ZIF-8 framework.The splitting of the asymmetric stretch of the CO_(2) into multiple peaks upon sorption indicate the presence of multiple environments,which could be a combination of free and physisorbed CO_(2) or simply multiple binding sites within the porous ionic liquid.A better understanding of gas sorption mechanisms in this unique material could lead to new porous ionic liquids with enhanced separations properties.展开更多
Electrocatalytic reduction of CO_2 is a promising route for energy storage and utilization. Herein we synthesized SnO_2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first ...Electrocatalytic reduction of CO_2 is a promising route for energy storage and utilization. Herein we synthesized SnO_2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first time. The SnO_2 and N-PC in the SnO_2@N-PC composites had exellent synergistic effect for electrocatalytic reduction of CO_2 to HCOOH. The Faradaic efficiency of HCOOH could be as high as 94.1% with a current density of 28.4 mA cm-2 in ionic liquid-MeCN system. The reaction mechanism was proposed on the basis of some control experiments. This work opens a new way to prepare composite electrode for electrochemical reduction of CO_2.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.22078135,21808092,21978119,22202088)。
文摘Porous ionic liquids have demonstrated excellent performance in the field of separation,attributed to their high specific surface area and efficient mass transfer.Herein,task-specific protic porous ionic liquids(PPILs)were prepared by employing a novel one-step coupling neutralization reaction strategy for extractive desulfurization.The single-extraction efficiency of PPILs reached 75.0%for dibenzothiophene.Moreover,adding aromatic hydrocarbon interferents resulted in a slight decrease in the extraction efficiency of PPILs(from 45.2%to 37.3%,37.9%,and 33.5%),indicating the excellent extraction selectivity of PPILs.The experimental measurements and density functional theory calculations reveal that the surface channels of porous structures can selectively capture dibenzothiophene by the stronger electrophilicity(Eint(HS surface channel/DBT)=-39.8 kcal mol^(-1)),and the multiple extraction sites of ion pairs can effectively enrich and transport dibenzothiophene from the oil phase into PPILs throughπ...π,C-H...πand hydrogen bonds interactions.Furthermore,this straightforward synthetic strategy can be employed in preparing porous liquids,offering new possibilities for synthesizing PPILs with tailored functionalities.
文摘Porous liquids,which are liquids with permanent porosity,have received significant attention as a new class of materials with the potential for far-reaching impacts in a variety of applications including gas separation.In this work,in situ Fourier transform infrared spectroscopy measurements were conducted to investigate the mechanism of carbon dioxide absorption in a porous ionic liquid consisting of ZIF-8 combined with 8,80-(3,6-dioxaoctane-1,8-diyl)bis(1,8-diazabicyclo[5.4.0]undec-7-en-8-ium)bis(trifluoromethanesulfonyl)imide([DBU-PEG][(Tf_(2)N)_(2)]).While the vibrational modes of the pure ionic liquid remain relatively unchanged,the incorporation of carbon dioxide leads to slight structural fluctuations in the ZIF-8 framework whether it is pure solid or as integrated into the porous ionic liquid.The analysis of the vibrational modes of the porous ionic liquid suggests that the interaction of the CO_(2) occurs more strongly with the ring structure of the ZIF-8 framework.The splitting of the asymmetric stretch of the CO_(2) into multiple peaks upon sorption indicate the presence of multiple environments,which could be a combination of free and physisorbed CO_(2) or simply multiple binding sites within the porous ionic liquid.A better understanding of gas sorption mechanisms in this unique material could lead to new porous ionic liquids with enhanced separations properties.
基金supported by the National Natural Science Foundation of China (21673248, 21533011)the National Key Research and Development Program of China (2017YFA0403102)Chinese Academy of Sciences (QYZDY-SSW-SLH013)
文摘Electrocatalytic reduction of CO_2 is a promising route for energy storage and utilization. Herein we synthesized SnO_2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first time. The SnO_2 and N-PC in the SnO_2@N-PC composites had exellent synergistic effect for electrocatalytic reduction of CO_2 to HCOOH. The Faradaic efficiency of HCOOH could be as high as 94.1% with a current density of 28.4 mA cm-2 in ionic liquid-MeCN system. The reaction mechanism was proposed on the basis of some control experiments. This work opens a new way to prepare composite electrode for electrochemical reduction of CO_2.