High surface area Nafion/SiO2 nanocomposites with nano-sized Nafion resin particles entrapped and dispersed within the highly porous silica matrix exhibited significantly enhanced activity, high selectivity and long-t...High surface area Nafion/SiO2 nanocomposites with nano-sized Nafion resin particles entrapped and dispersed within the highly porous silica matrix exhibited significantly enhanced activity, high selectivity and long-term stability for the alkylation of benzene with linear C9-C13 alkenes owing to the increased accessibility of Nafion resin-based acid sites to reactants.展开更多
Hydrophilicity is critical in Nafion membranes during fuel cell operation as insufficient membrane hydration leads to brittle behavior and a drop in proton conductivity.The incorporation of APTS(3-(aminopro pyl)trieth...Hydrophilicity is critical in Nafion membranes during fuel cell operation as insufficient membrane hydration leads to brittle behavior and a drop in proton conductivity.The incorporation of APTS(3-(aminopro pyl)triethoxysilane)into exfoliated graphene oxide(EGO)by covalent functionalization to be used as filler into Nafion membranes allows higher hydrophilicity for these membranes.This is associated with promoting hydroxyl,carbonyl,siloxane,silane,and amine groups within the EGO-APTS matrix.The incorporation of these materials as Fuel Cell MEAs leads to a significant reduction of the ohmic resistance measured at high frequency resistance(HFR)in electrochemical impedance spectroscopy(EIS)experiments and achieves maximum power densities of 1.33 W cm-2at 60℃ at 100%RH(APTS-EGO,0.2 wt%)and1.33 W cm-2at 60℃ at 70%RH(APTS-EGO,0.3 wt%),which represents an improvement of 190%compared to the commercial Nafion 212 when utilizing low humidification conditions(70%).Moreover,the as-synthesized membrane utilizes lower Nafion ionomer mass,which,in conjunction with the excellent cell performance,has the potential to decrease the cost of the membrane from 87 to 80£/W as well as a reduction of fluorinated compounds within the membrane.展开更多
Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO2electrolysis.Here...Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO2electrolysis.Herein,the key roles of Nafion for CO2RR were systematically studied on Cu nanoparticles(NPs)electrocatalyst.We found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H2O from electrolyte to Cu NPs,and increase the CO2concentration at electrocatalyst interface for enhancing the CO2mass transfer process,but also activate CO2molecule by Lewis acid-base interaction between Nafion and CO2to accelerate the formation of*CO,which favor of C–C coupling for boosting C2product generation.Owing to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C2products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology reconstruction.Thus,this work provides insights into the impact of Nafion on electrocatalytic CO2RR performance.展开更多
Nafion/TiO2 composite membranes were prepared by in-situ chemical reaction method using Ti(OC4H9)4 and Nafion 117 as raw materials. The membranes were characterized by UV, FTIR-ATR and XRD, respectively. Methanol perm...Nafion/TiO2 composite membranes were prepared by in-situ chemical reaction method using Ti(OC4H9)4 and Nafion 117 as raw materials. The membranes were characterized by UV, FTIR-ATR and XRD, respectively. Methanol permeability and water uptake were investigated as a function of TiO2 contents. The conductivity of the membranes was measured under water vapor pressure (2.644 7 kPa) or in dry atmospheres. The XRD results showed that the titanium dioxide in Nafion membranes were crystallized in anatase phase with an average crys- taline diameter of 3.0 nm. The water uptake of the composite membranes was larger than that of the pure Nafion○ membrane when the TiO2 loading was within 14wt%. The methanol permeability of the membrane decreased as the TiO2 loading increased. The addition of 3wt% TiO2 to Nafion○ membranes improved the conductivity in dry measurement conditions. The proton conductivity of the composite membrane increased greatly after the hy- drothermal treatment at 160 ℃ for 2 hours.展开更多
摘要High surface area Nafion/SiO2 nanocomposites with nano-sized Nafion resin particles entrapped and dispersed within the highly porous silica matrix exhibited significantly enhanced activity, high selectivity and long-term stability for the alkylation of benzene with linear C9-C13 alkenes owing to the increased accessibility of Nafion resin-based acid sites to reactants.
基金financially supported by the UK Research Council EPRSC EP/W03395X/1the Program grant SynHiSel EP/V047078/1the Hydrogen and Fuel Cells Hub(H2FC SUPERGEN)EP/P024807/1。
摘要Hydrophilicity is critical in Nafion membranes during fuel cell operation as insufficient membrane hydration leads to brittle behavior and a drop in proton conductivity.The incorporation of APTS(3-(aminopro pyl)triethoxysilane)into exfoliated graphene oxide(EGO)by covalent functionalization to be used as filler into Nafion membranes allows higher hydrophilicity for these membranes.This is associated with promoting hydroxyl,carbonyl,siloxane,silane,and amine groups within the EGO-APTS matrix.The incorporation of these materials as Fuel Cell MEAs leads to a significant reduction of the ohmic resistance measured at high frequency resistance(HFR)in electrochemical impedance spectroscopy(EIS)experiments and achieves maximum power densities of 1.33 W cm-2at 60℃ at 100%RH(APTS-EGO,0.2 wt%)and1.33 W cm-2at 60℃ at 70%RH(APTS-EGO,0.3 wt%),which represents an improvement of 190%compared to the commercial Nafion 212 when utilizing low humidification conditions(70%).Moreover,the as-synthesized membrane utilizes lower Nafion ionomer mass,which,in conjunction with the excellent cell performance,has the potential to decrease the cost of the membrane from 87 to 80£/W as well as a reduction of fluorinated compounds within the membrane.
基金financially supported by the Natural Science Foundation of Guangdong Province (2022A1515012359)the National Natural Science Foundation of China (21902121)+1 种基金the STU Scientific Research Foundation for Talents (NTF21020)the 2020 Li Ka Shing Foundation Cross-Disciplinary Research Grant (2020LKSFG09A)。
摘要Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO2electrolysis.Herein,the key roles of Nafion for CO2RR were systematically studied on Cu nanoparticles(NPs)electrocatalyst.We found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H2O from electrolyte to Cu NPs,and increase the CO2concentration at electrocatalyst interface for enhancing the CO2mass transfer process,but also activate CO2molecule by Lewis acid-base interaction between Nafion and CO2to accelerate the formation of*CO,which favor of C–C coupling for boosting C2product generation.Owing to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C2products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology reconstruction.Thus,this work provides insights into the impact of Nafion on electrocatalytic CO2RR performance.
摘要Nafion/TiO2 composite membranes were prepared by in-situ chemical reaction method using Ti(OC4H9)4 and Nafion 117 as raw materials. The membranes were characterized by UV, FTIR-ATR and XRD, respectively. Methanol permeability and water uptake were investigated as a function of TiO2 contents. The conductivity of the membranes was measured under water vapor pressure (2.644 7 kPa) or in dry atmospheres. The XRD results showed that the titanium dioxide in Nafion membranes were crystallized in anatase phase with an average crys- taline diameter of 3.0 nm. The water uptake of the composite membranes was larger than that of the pure Nafion○ membrane when the TiO2 loading was within 14wt%. The methanol permeability of the membrane decreased as the TiO2 loading increased. The addition of 3wt% TiO2 to Nafion○ membranes improved the conductivity in dry measurement conditions. The proton conductivity of the composite membrane increased greatly after the hy- drothermal treatment at 160 ℃ for 2 hours.