Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high...Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high oxygen evolution potential(OEP)and considerable barrier to generating reactive oxygen species(ROS).Herein,an innovative TNAs/SnO_(2)/PEDOT/Fe(Ⅲ)-RuO_(2) multilayer electrode was synthesized by utilizing a PEDOT-coated SnO_(2) interlayer as a supportive framework to combine Fe-doped amorphous RuO_(2) catalytic layer with TiO_(2) nanotube array substrate.Such electrode exhibited high activity and sta-bility for the oxidation of As(Ⅲ)to As(V)due to the large surface area provided by the TiO_(2) nanotube arrays and the SnO_(2)/PEDOT interlayer for facilitating the growth of the catalytic layer.The electrochem-ically active surface area of the electrode reached as high as 31.7 mF/cm^(2).Impressively,the doping of Fe into RuO_(2) layer led to a remarkable increase in the OEP value to 3.12 V,which boosted the indirect oxidation process mediated by ROS at a lower potential to achieve the As(Ⅲ)oxidation ratio of 98.5%.DFT calculations revealed that the Fe-doped amorphous RuO_(2) weakened the adsorption strength of·OH and.SO4-intermediates and lowered the energy barrier for generating ROS.Combined with ESR results,the formation of·OH and·SC4-with strong oxidizing properties was fully verified,providing further evi-dence for the involvement of ROS as the main mediator of the oxidation mechanism of As(Ⅲ).This work may provide valuable perspectives into the design of catalytic layer structures and heteroatom doping modifications for composite-coated electrodes.展开更多
The densities and surface tensions of [Bmim][TFO]/H2SO4, [Hmim][TFO]/H2SO4 and [Omim][TFO]/H2SO4 binary mixtures were measured by pycnometer and Wilhelmy plate method respectively. The results show that densities and ...The densities and surface tensions of [Bmim][TFO]/H2SO4, [Hmim][TFO]/H2SO4 and [Omim][TFO]/H2SO4 binary mixtures were measured by pycnometer and Wilhelmy plate method respectively. The results show that densities and surface tensions of the mixtures decreased monotonously with increasing temperatures and increasing ionic liquid （IL） molar fraction. IL with longer alkyl side-chain length brings a lower density and a smaller surface tension to the ILs/H2SO4 binary mixtures. The densities and surface tensions of the mixtures are fitted well by Jouyban-Acree （JAM） model and LWW model respectively. Redlich-Kister （R-K）equation and modified Redlich-Kister （R-K） equation describe the excess molar volumes and excess surface tensions of the mixtures well respectively. Adding a small amount of ILs （XIL 〈 0.1 ） into sulfuric acid brings an obvious decrease to the density and the surface tension. The results imply that the densities and surface tensions of IL5/H2SO4 binary mixtures can be modulated by changing the IL dosage or tailoring the IL structure.展开更多
Oxidative coupling of methane is a direct way to obtain C2 hydrocarbon, and Mn-Na-W/SiO2 catalyst is the most promising among all the catalysts. The 2%Mn/5%Na2WO4/SiO2 catalyst was prepared by the incipient wetness im...Oxidative coupling of methane is a direct way to obtain C2 hydrocarbon, and Mn-Na-W/SiO2 catalyst is the most promising among all the catalysts. The 2%Mn/5%Na2WO4/SiO2 catalyst was prepared by the incipient wetness impregnation method. A 7-step heterogeneous reaction model of the oxidative coupling of methane to C2 hydrocarbons was conducted by co-feeding methane and oxygen at a total pressure of 1 bar over the catalyst. The kinetic measurements were carried out in a micro-catalytic fixed bed reactor. The kinetic data were obtained at the appropriate range of reaction conditions （4 kPa〈Po2 〈20 kPa, 20 kPa〈PcH4〈80 kPa, 800 ℃〈T〈900℃）. The proposed reaction kinetic scheme consists of three primary and four consecutive reaction steps. The conversions of hydrocarbons and carbon oxides were evaluated by applying Langmuir-Hinshelwood type rate equations. Power-law rate equation was applied only for the water-gas shift reaction. In addition, the effects of operating conditions on the reaction rate were studied. The proposed kinetic model can predict the conversion of methane and oxygen as well as the yield of C2 hydrocarbons and carbon oxides with an average accuracy of ± 15%.展开更多
The complicated reaction mechanism and the character of competitive reactions lead to a stringent requirement for the catalyst of C_4 alkylation process. Due to their unique properties, ionic liquids(ILs) are thought ...The complicated reaction mechanism and the character of competitive reactions lead to a stringent requirement for the catalyst of C_4 alkylation process. Due to their unique properties, ionic liquids(ILs) are thought to be new potential acid catalysts for C_4 alkylation. An analysis of the regular and modified chloroaluminate ILs, novel Br?nsted ILs and composite ILs used in isobutane/butene alkylation shows that the use of either ILs or ILs coupled with mineral acid as homogeneous catalysts can help to greatly adjust the acid strength. By modifying the structural parameters of the cations and anions of the ILs, the solubility of the reactants could also be adjusted, which in turn displays a positive effect on improving the activity of ILs. Immobilization of ILs is an effective way to modulate the surface adsorption/desorption properties and acid strength distribution of the solid acid catalysts. Such a process has a tremendous potential to reduce the deactivation of catalyst and enhance the activity of the solid acid catalyst. The development of novel acid catalysts for C_4 alkylation is a comprehensive consideration of acid strength and its distribution, interfacial properties and transport characteristics.展开更多
Ni/α-Al2O3 catalysts were found to be active in the temperature range 600 ～ 900℃ for both CO2 reforming and partial oxidation of methane.The effects of Ni loading,reaction temperature and feed gas ratio for the com...Ni/α-Al2O3 catalysts were found to be active in the temperature range 600 ～ 900℃ for both CO2 reforming and partial oxidation of methane.The effects of Ni loading,reaction temperature and feed gas ratio for the combination of CO2 reforming and partial oxidation of CH4 over Ni/α-Al2O3 were investigated.Catalysts of xwt%Ni/α-Al2O3（x=2.5,5,8 and 12） were prepared by wet impregnating the calcined support with a solution of nickel nitrate.XRD patterns and activity tests have verified that the 5wt%Ni/α-Al2O3 was the most active catalyst,as compared with the other prepared catalyst samples.An increase of the Ni loading to more than 5wt% led to a reduction in the Ni dispersion.In addition,by combining the endothermic carbon dioxide reforming reaction with the exothermic partial oxidation reaction,the loss of catalyst activity with time on stream was reduced with the amount of oxygen added to the feed.展开更多
Adsorption properties of an adsorbent or a catalyst towards adsorbates are crucial in the process of adsorption separation or catalytic reaction. Surface morphology and structure of adsorbents have a significant impac...Adsorption properties of an adsorbent or a catalyst towards adsorbates are crucial in the process of adsorption separation or catalytic reaction. Surface morphology and structure of adsorbents have a significant impact on the adsorption properties. In this study, a novel acidic ionic liquid, 1-butyl-3-(triethoxysilylpropyl)imidazolium hydrogen sulfate(i.e., [BTPIm][HSO_4]), was synthesized and subsequently grafted onto the MCM-36 zeolite for the regulation of its adsorption properties towards isobutane and 1-butene. The resultant [BTPIm][HSO_4]-immobilized MCM-36(i.e., MCM-36-IL) was characterized by FT-IR, XPS, XRD, SEM, TG/DTG and N_2 adsorption–desorption measurement. It was found that the specific surface area, micropore volume and mesopore volume of the MCM-36 support underwent a reduction upon the immobilization of ionic liquid,while the surface density of acid increased from 0.0014 to 0.0035 mmol·m^(-2). The adsorption capacity of isobutane and 1-butene on the MCM-36-IL was determined by a static volumetric method. Results demonstrated that the interaction between isobutane and MCM-36-IL was enhanced and the interaction between 1-butene and MCM-36-IL was reduced. As a result, a tunable adsorption ratio of isobutane/1-butene on MCM-36 was achieved.With the increase in surface density of acid and the tunable adsorption ratio of isobutane and 1-butene on the functionalized MCM-36, the acidic ionic liquid-immobilized zeolites are beneficial to obtain an improved reaction yield and a prolonged catalyst life in the reactions catalyzed by solid acid.展开更多
Superhydrophobic coating has been widely studied for its great applicational potential, such as for corrosion protection of magnesium alloys while it has been restrained by expensive materials, sophisticated preparati...Superhydrophobic coating has been widely studied for its great applicational potential, such as for corrosion protection of magnesium alloys while it has been restrained by expensive materials, sophisticated preparation process and infirm rough structures. In this study, the electrochemical method was adopted by using a two-electrode system for rapid hydrophobic modification to obtain superhydrophobic kaolin.By mixing the modified superhydrophobic kaolin with commercial epoxy resin and polydimethylsiloxane glue, a paint can be formed and easily used on various substrates for preparation of superhydrophobic coating via spraying method. The influence factors on wettability of the modified kaolin and the mixing ratio of each component of the coating were explored. Also, the wettability, durability and anticorrosion of the prepared coating were evaluated comprehensively. The coating was able to maintain superhydrophobic after immersed in HCl solution at pH 1, the NaOH solution at pH 14, and 3.5 wt.% NaCl solution for 16, 21, 30 days, respectively. In addition, the coating exhibited 4A grade adhesion, high hydrophobicity after abraded for 200 cycles on a 600-mesh sandpaper with 100 g weight, and 99.86% anticorrosion efficiency after soaked in 3.5 wt.% NaCl solution for 20 days, demonstrating a good robustness and anti-corrosion property. Furthermore, the coating showed good transparency, flexibility and was easy to make in a large scale by the spraying method, which is of great significance to promote the practical application of superhydrophobic coatings and the anticorrosion Mg alloys.展开更多
Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials.Herein,we propose a rapid and simple methodology,flame synthesis,as an effective preparation strategy for inc...Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials.Herein,we propose a rapid and simple methodology,flame synthesis,as an effective preparation strategy for incorporating high-valence metal ions(Ti^(4+),Sn^(4+),and Zr^(4+))into ultrasmall Fe_(2)O_(3)on carbon nanotube support(i.e.,M-FeO-CNT).The resulting materials exhibit not only a boosted Na+adsorption as shown by density functional theory(DFT)calculations,but also display an increased oxygen deficiency.The electrochemical activity and charge transfer efficiency of Fe 2 O 3 can be improved by reasonably sub-stituting Fe 3+with Ti^(4+),Sn^(4+),and Zr^(4+).The electrochemical investigation of Ti-doped Fe 2 O 3(Ti-FeO-CNT)electrode demonstrates a splendid specific capacitance of 1.25 F cm^(−2)at 1 mA cm^(−2)in 1 M Na_(2)SO_(4).This is significantly higher as compared to the capacitance of 0.48 F cm^(−2).Flexible solid-state asymmetric su-percapacitor Ti-FeO-CNT//MnO_(2)is verified with operating voltage of 2.0 V and stability over 3000 cycles,and delivers a high energy density of 2.14 mWh cm^(−3)at power density of 25 mW cm−3.The flame synthesis is expected to be widely applicable for the preparation of high-valence metal ions doped nanosized Fe_(2)O_(3)functionalized materials,thus opening up new avenues for energy and catalysis research.展开更多
Designing of hetero-atomic doped carbon-based systems through pyrolysis of abundant element organic precursors is a novel approach to construct rational porous carbon materials.Herein,a highly-cross-linked triazine po...Designing of hetero-atomic doped carbon-based systems through pyrolysis of abundant element organic precursors is a novel approach to construct rational porous carbon materials.Herein,a highly-cross-linked triazine polymer is employed to fabricate N,P co-doped porous carbon(A-TDP-12)with tunable active nitrogen in the carbon framework for simultaneous enhancement of CO_(2) capture capability and Supercapacitance(SC).The synthesized A-TDP-12 possesses a typical hierarchically porous framework(micro-pores and meso-pores)with a large surface area(1332 m^(2) g^(-1))and a rich content of N(7.89 at.%)and P(0.74 at.%).It delivers a CO_(2) adsorption capacity of 1.52 and 5.68 mmol g^(-1) at 1 and 5 bar,respectively,with almost no decay after successive 8 recycles.In 6 M KOH aqueous electrolyte,A-TDP-12 exhibits a superior specific capacitance of 172.7 F g^(-1) at a current density of 1 A g^(-1).Even at a high current density of 10 A g^(-1),80%of its initial capacity still remains.This work not only offers a novel strategy for fabricating promising adsorbents and electrodes for CO_(2) uptake and SCs,but also provides new insights into design of porous carbon material for related applications.展开更多
The adsorption ratio of isobutane/1-butene on the catalyst surface is one of the most important factors for the C4 alkylation process. Regulation of isobutane/1-butene adsorption ratio on the zeolite-supported acid ca...The adsorption ratio of isobutane/1-butene on the catalyst surface is one of the most important factors for the C4 alkylation process. Regulation of isobutane/1-butene adsorption ratio on the zeolite-supported acid catalyst is a big challenge for catalyst preparation. To regulate the isobutane/1-butene adsorption ratio, four types of ionic liquid （i.e., IL） with different alkyl chain lengths and different acid group numbers were synthesized and were subsequently immobilized onto the MCM-22 zeolite. The as-synthesized IL-immobilized MCM-22 （i.e., MCM-22-IL） was characterized by FT1R, TGA, BET, XPS and XRD, and their adsorption capacities and adsorption molar ratios of isobutane to l-butene （I/O） were investigated to correlate with surface features of MCM-22-IL Results showed that the immobilization of ILs led to a decrease of specific surface area and pore volume. But the surface density of acid groups was increased and the adsorption molar ratio of isobutane/1-butene （I/O） was significantly im- proved by the immobilization of ionic liquids. The adsorption molar ratio of I/O is substantially improved from 0.75 to above 0.9 at 300 kPa upon immobilizing ILs. Although the alkyl chain length oflLs was found to have little effect on the adsorption molar ratio of I/O, the increase of acid group numbers led to a dramatic decrease in the adsorption I/O ratio. The results illustrated that immobilizing ionic liquids is an effective way to modify the textural, chemical and morphological properties of MCM-22. Accordingly, the immobilization of ionic liquids provides a novel and a feasible way to regulate the adsorption I/O ratio on an adsorbent or a solid catalyst.展开更多
基金National Natural Science Foundation of China(No.21978182)。
文摘Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high oxygen evolution potential(OEP)and considerable barrier to generating reactive oxygen species(ROS).Herein,an innovative TNAs/SnO_(2)/PEDOT/Fe(Ⅲ)-RuO_(2) multilayer electrode was synthesized by utilizing a PEDOT-coated SnO_(2) interlayer as a supportive framework to combine Fe-doped amorphous RuO_(2) catalytic layer with TiO_(2) nanotube array substrate.Such electrode exhibited high activity and sta-bility for the oxidation of As(Ⅲ)to As(V)due to the large surface area provided by the TiO_(2) nanotube arrays and the SnO_(2)/PEDOT interlayer for facilitating the growth of the catalytic layer.The electrochem-ically active surface area of the electrode reached as high as 31.7 mF/cm^(2).Impressively,the doping of Fe into RuO_(2) layer led to a remarkable increase in the OEP value to 3.12 V,which boosted the indirect oxidation process mediated by ROS at a lower potential to achieve the As(Ⅲ)oxidation ratio of 98.5%.DFT calculations revealed that the Fe-doped amorphous RuO_(2) weakened the adsorption strength of·OH and.SO4-intermediates and lowered the energy barrier for generating ROS.Combined with ESR results,the formation of·OH and·SC4-with strong oxidizing properties was fully verified,providing further evi-dence for the involvement of ROS as the main mediator of the oxidation mechanism of As(Ⅲ).This work may provide valuable perspectives into the design of catalytic layer structures and heteroatom doping modifications for composite-coated electrodes.
基金Supported by the National Natural Science Foundation of China(21576168,21276163)
文摘The densities and surface tensions of [Bmim][TFO]/H2SO4, [Hmim][TFO]/H2SO4 and [Omim][TFO]/H2SO4 binary mixtures were measured by pycnometer and Wilhelmy plate method respectively. The results show that densities and surface tensions of the mixtures decreased monotonously with increasing temperatures and increasing ionic liquid （IL） molar fraction. IL with longer alkyl side-chain length brings a lower density and a smaller surface tension to the ILs/H2SO4 binary mixtures. The densities and surface tensions of the mixtures are fitted well by Jouyban-Acree （JAM） model and LWW model respectively. Redlich-Kister （R-K）equation and modified Redlich-Kister （R-K） equation describe the excess molar volumes and excess surface tensions of the mixtures well respectively. Adding a small amount of ILs （XIL 〈 0.1 ） into sulfuric acid brings an obvious decrease to the density and the surface tension. The results imply that the densities and surface tensions of IL5/H2SO4 binary mixtures can be modulated by changing the IL dosage or tailoring the IL structure.
基金This work was financially supported by the Research Department of Iran University of Science and Technology
文摘Oxidative coupling of methane is a direct way to obtain C2 hydrocarbon, and Mn-Na-W/SiO2 catalyst is the most promising among all the catalysts. The 2%Mn/5%Na2WO4/SiO2 catalyst was prepared by the incipient wetness impregnation method. A 7-step heterogeneous reaction model of the oxidative coupling of methane to C2 hydrocarbons was conducted by co-feeding methane and oxygen at a total pressure of 1 bar over the catalyst. The kinetic measurements were carried out in a micro-catalytic fixed bed reactor. The kinetic data were obtained at the appropriate range of reaction conditions （4 kPa〈Po2 〈20 kPa, 20 kPa〈PcH4〈80 kPa, 800 ℃〈T〈900℃）. The proposed reaction kinetic scheme consists of three primary and four consecutive reaction steps. The conversions of hydrocarbons and carbon oxides were evaluated by applying Langmuir-Hinshelwood type rate equations. Power-law rate equation was applied only for the water-gas shift reaction. In addition, the effects of operating conditions on the reaction rate were studied. The proposed kinetic model can predict the conversion of methane and oxygen as well as the yield of C2 hydrocarbons and carbon oxides with an average accuracy of ± 15%.
基金Supported by the National Natural Science Foundation of China(21276163,21576168)
文摘The complicated reaction mechanism and the character of competitive reactions lead to a stringent requirement for the catalyst of C_4 alkylation process. Due to their unique properties, ionic liquids(ILs) are thought to be new potential acid catalysts for C_4 alkylation. An analysis of the regular and modified chloroaluminate ILs, novel Br?nsted ILs and composite ILs used in isobutane/butene alkylation shows that the use of either ILs or ILs coupled with mineral acid as homogeneous catalysts can help to greatly adjust the acid strength. By modifying the structural parameters of the cations and anions of the ILs, the solubility of the reactants could also be adjusted, which in turn displays a positive effect on improving the activity of ILs. Immobilization of ILs is an effective way to modulate the surface adsorption/desorption properties and acid strength distribution of the solid acid catalysts. Such a process has a tremendous potential to reduce the deactivation of catalyst and enhance the activity of the solid acid catalyst. The development of novel acid catalysts for C_4 alkylation is a comprehensive consideration of acid strength and its distribution, interfacial properties and transport characteristics.
文摘Ni/α-Al2O3 catalysts were found to be active in the temperature range 600 ～ 900℃ for both CO2 reforming and partial oxidation of methane.The effects of Ni loading,reaction temperature and feed gas ratio for the combination of CO2 reforming and partial oxidation of CH4 over Ni/α-Al2O3 were investigated.Catalysts of xwt%Ni/α-Al2O3（x=2.5,5,8 and 12） were prepared by wet impregnating the calcined support with a solution of nickel nitrate.XRD patterns and activity tests have verified that the 5wt%Ni/α-Al2O3 was the most active catalyst,as compared with the other prepared catalyst samples.An increase of the Ni loading to more than 5wt% led to a reduction in the Ni dispersion.In addition,by combining the endothermic carbon dioxide reforming reaction with the exothermic partial oxidation reaction,the loss of catalyst activity with time on stream was reduced with the amount of oxygen added to the feed.
基金Supported by the National Natural Science Foundation of China(No.21276163,and No.21576168)
文摘Adsorption properties of an adsorbent or a catalyst towards adsorbates are crucial in the process of adsorption separation or catalytic reaction. Surface morphology and structure of adsorbents have a significant impact on the adsorption properties. In this study, a novel acidic ionic liquid, 1-butyl-3-(triethoxysilylpropyl)imidazolium hydrogen sulfate(i.e., [BTPIm][HSO_4]), was synthesized and subsequently grafted onto the MCM-36 zeolite for the regulation of its adsorption properties towards isobutane and 1-butene. The resultant [BTPIm][HSO_4]-immobilized MCM-36(i.e., MCM-36-IL) was characterized by FT-IR, XPS, XRD, SEM, TG/DTG and N_2 adsorption–desorption measurement. It was found that the specific surface area, micropore volume and mesopore volume of the MCM-36 support underwent a reduction upon the immobilization of ionic liquid,while the surface density of acid increased from 0.0014 to 0.0035 mmol·m^(-2). The adsorption capacity of isobutane and 1-butene on the MCM-36-IL was determined by a static volumetric method. Results demonstrated that the interaction between isobutane and MCM-36-IL was enhanced and the interaction between 1-butene and MCM-36-IL was reduced. As a result, a tunable adsorption ratio of isobutane/1-butene on MCM-36 was achieved.With the increase in surface density of acid and the tunable adsorption ratio of isobutane and 1-butene on the functionalized MCM-36, the acidic ionic liquid-immobilized zeolites are beneficial to obtain an improved reaction yield and a prolonged catalyst life in the reactions catalyzed by solid acid.
基金the financial support of the National Natural Science Foundation of China (Grant No. 21978182)。
文摘Superhydrophobic coating has been widely studied for its great applicational potential, such as for corrosion protection of magnesium alloys while it has been restrained by expensive materials, sophisticated preparation process and infirm rough structures. In this study, the electrochemical method was adopted by using a two-electrode system for rapid hydrophobic modification to obtain superhydrophobic kaolin.By mixing the modified superhydrophobic kaolin with commercial epoxy resin and polydimethylsiloxane glue, a paint can be formed and easily used on various substrates for preparation of superhydrophobic coating via spraying method. The influence factors on wettability of the modified kaolin and the mixing ratio of each component of the coating were explored. Also, the wettability, durability and anticorrosion of the prepared coating were evaluated comprehensively. The coating was able to maintain superhydrophobic after immersed in HCl solution at pH 1, the NaOH solution at pH 14, and 3.5 wt.% NaCl solution for 16, 21, 30 days, respectively. In addition, the coating exhibited 4A grade adhesion, high hydrophobicity after abraded for 200 cycles on a 600-mesh sandpaper with 100 g weight, and 99.86% anticorrosion efficiency after soaked in 3.5 wt.% NaCl solution for 20 days, demonstrating a good robustness and anti-corrosion property. Furthermore, the coating showed good transparency, flexibility and was easy to make in a large scale by the spraying method, which is of great significance to promote the practical application of superhydrophobic coatings and the anticorrosion Mg alloys.
基金supported by the National Natu-ral Science Foundation of China(No.21978182)the Miaozi Project in Science and Technology Innovation Program of Sichuan Province(No.21-YCG021).
文摘Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials.Herein,we propose a rapid and simple methodology,flame synthesis,as an effective preparation strategy for incorporating high-valence metal ions(Ti^(4+),Sn^(4+),and Zr^(4+))into ultrasmall Fe_(2)O_(3)on carbon nanotube support(i.e.,M-FeO-CNT).The resulting materials exhibit not only a boosted Na+adsorption as shown by density functional theory(DFT)calculations,but also display an increased oxygen deficiency.The electrochemical activity and charge transfer efficiency of Fe 2 O 3 can be improved by reasonably sub-stituting Fe 3+with Ti^(4+),Sn^(4+),and Zr^(4+).The electrochemical investigation of Ti-doped Fe 2 O 3(Ti-FeO-CNT)electrode demonstrates a splendid specific capacitance of 1.25 F cm^(−2)at 1 mA cm^(−2)in 1 M Na_(2)SO_(4).This is significantly higher as compared to the capacitance of 0.48 F cm^(−2).Flexible solid-state asymmetric su-percapacitor Ti-FeO-CNT//MnO_(2)is verified with operating voltage of 2.0 V and stability over 3000 cycles,and delivers a high energy density of 2.14 mWh cm^(−3)at power density of 25 mW cm−3.The flame synthesis is expected to be widely applicable for the preparation of high-valence metal ions doped nanosized Fe_(2)O_(3)functionalized materials,thus opening up new avenues for energy and catalysis research.
基金supported by the National Natural Science Foundation of China (21978182)
文摘Designing of hetero-atomic doped carbon-based systems through pyrolysis of abundant element organic precursors is a novel approach to construct rational porous carbon materials.Herein,a highly-cross-linked triazine polymer is employed to fabricate N,P co-doped porous carbon(A-TDP-12)with tunable active nitrogen in the carbon framework for simultaneous enhancement of CO_(2) capture capability and Supercapacitance(SC).The synthesized A-TDP-12 possesses a typical hierarchically porous framework(micro-pores and meso-pores)with a large surface area(1332 m^(2) g^(-1))and a rich content of N(7.89 at.%)and P(0.74 at.%).It delivers a CO_(2) adsorption capacity of 1.52 and 5.68 mmol g^(-1) at 1 and 5 bar,respectively,with almost no decay after successive 8 recycles.In 6 M KOH aqueous electrolyte,A-TDP-12 exhibits a superior specific capacitance of 172.7 F g^(-1) at a current density of 1 A g^(-1).Even at a high current density of 10 A g^(-1),80%of its initial capacity still remains.This work not only offers a novel strategy for fabricating promising adsorbents and electrodes for CO_(2) uptake and SCs,but also provides new insights into design of porous carbon material for related applications.
基金Supported by the National Natural Science Foundation of China(21576168,21276163)
文摘The adsorption ratio of isobutane/1-butene on the catalyst surface is one of the most important factors for the C4 alkylation process. Regulation of isobutane/1-butene adsorption ratio on the zeolite-supported acid catalyst is a big challenge for catalyst preparation. To regulate the isobutane/1-butene adsorption ratio, four types of ionic liquid （i.e., IL） with different alkyl chain lengths and different acid group numbers were synthesized and were subsequently immobilized onto the MCM-22 zeolite. The as-synthesized IL-immobilized MCM-22 （i.e., MCM-22-IL） was characterized by FT1R, TGA, BET, XPS and XRD, and their adsorption capacities and adsorption molar ratios of isobutane to l-butene （I/O） were investigated to correlate with surface features of MCM-22-IL Results showed that the immobilization of ILs led to a decrease of specific surface area and pore volume. But the surface density of acid groups was increased and the adsorption molar ratio of isobutane/1-butene （I/O） was significantly im- proved by the immobilization of ionic liquids. The adsorption molar ratio of I/O is substantially improved from 0.75 to above 0.9 at 300 kPa upon immobilizing ILs. Although the alkyl chain length oflLs was found to have little effect on the adsorption molar ratio of I/O, the increase of acid group numbers led to a dramatic decrease in the adsorption I/O ratio. The results illustrated that immobilizing ionic liquids is an effective way to modify the textural, chemical and morphological properties of MCM-22. Accordingly, the immobilization of ionic liquids provides a novel and a feasible way to regulate the adsorption I/O ratio on an adsorbent or a solid catalyst.
