Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms we...Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms were of Brunauer type I and well correlated with Langmuir-Freundlich model. After sodium ions exchange, the adsorption amounts of three adsorbates increased, while the increase magnitude of CO2 adsorption capacity was much higher than that of CH4 and N2. The selectivities of CO2 over CH4 and CO2 over N2 enhanced after sodium exchange. Also, the initial heat of adsorption data implied a stronger interaction of CO2 molecules with Na+ ions in Naβ . These results can be attributed to the larger electrostatic interaction of CO2 with extraframework cations in zeolites. However, Naβ showed a decrease in the selectivity of CH4 over N2, which can be ascribed to the moderate affinity of N2 with Naβ. The variation of isosteric heats of adsorption as a function of loading indicates that the adsorption of CO2 in Naβ presents an energetically heterogeneous profile. On the contrary, the adsorption of CH4 was found to be essentially homogeneous, which suggests the dispersion interaction between CH4 and lattice oxygen atoms, and such interaction does not depend on the exchangeable cations of zeolite.展开更多
用相同摩尔浓度的硝酸铵,柠檬酸以及柠檬酸铵溶液对Naβ沸石进行改性处理得到Hβ沸石;采用XRD、XRF、FT-IR、27Al MAS NMR和29Si MAS NMR等表征手段进行分析。结果表明,采用含羟基的柠檬酸或柠檬酸铵对Naβ沸石进行改性处理,不但可以提...用相同摩尔浓度的硝酸铵,柠檬酸以及柠檬酸铵溶液对Naβ沸石进行改性处理得到Hβ沸石;采用XRD、XRF、FT-IR、27Al MAS NMR和29Si MAS NMR等表征手段进行分析。结果表明,采用含羟基的柠檬酸或柠檬酸铵对Naβ沸石进行改性处理,不但可以提高样品结晶度还可以有效限制骨架铝的脱除;经柠檬酸或柠檬酸铵改性可以使Naβ中的Al(S4R,SiteA)转化成Al(S6R,SiteB),而硝酸铵改性的Naβ沸石中只发现一种骨架四面体;还发现硝酸铵和柠檬酸铵改性Naβ沸石后,少量的骨架铝转化为非骨架铝并存在于孔道内,而经过柠檬酸改性后,这部分非骨架铝被带出孔道。展开更多
用相同物质的量浓度的硝酸铵、柠檬酸以及柠檬酸铵溶液对Naβ沸石进行改性处理得到Hβ沸石;采用XRD、XRF、FT-IR、27Al MAS NMR和29Si MAS NMR等表征手段进行分析。结果表明,采用含羟基的柠檬酸或柠檬酸铵对Naβ沸石进行改性处理,不但...用相同物质的量浓度的硝酸铵、柠檬酸以及柠檬酸铵溶液对Naβ沸石进行改性处理得到Hβ沸石;采用XRD、XRF、FT-IR、27Al MAS NMR和29Si MAS NMR等表征手段进行分析。结果表明,采用含羟基的柠檬酸或柠檬酸铵对Naβ沸石进行改性处理,不但可以提高样品结晶度还可以有效限制骨架铝的脱除;经柠檬酸或柠檬酸铵改性可以使Naβ中的Al(S4R,SiteA)转化成Al(S6R,SiteB),而硝酸铵改性的Naβ沸石中只发现一种骨架四面体;还发现硝酸铵和柠檬酸铵改性Naβ沸石后,少量的骨架铝转化为非骨架铝并存在于孔道内,而经过柠檬酸改性后,这部分非骨架铝被带出孔道。展开更多
1.IntroductionDunn and Farrington[1]found that theNa ion in Naβ″-alumina single crystal canbe exchanged completely or partially withGd;,Nd;,Eu;,Yb;,Sm;,Tb;,Dy;,Bi;and Pr;ions,but no reports havebeen published about... 1.IntroductionDunn and Farrington[1]found that theNa ion in Naβ″-alumina single crystal canbe exchanged completely or partially withGd;,Nd;,Eu;,Yb;,Sm;,Tb;,Dy;,Bi;and Pr;ions,but no reports havebeen published about the ion exchange reac-tion between La3+ and Naβ″-alumina.If anion exchanged polycrystalline β″-alumina isavailable and its ionic conductivity is highenough to be applied as a solid electrolyte inthe galvanic cell,it can be used in various展开更多
基金supported by the Doctoral Program of Higher Education(Project 200402910050)the Program for Changiiang Scholars and Innovative Research Team in University(No.IRT0732)Major Basic Research Project of Natural Science Foundation of Jiangsu Province Colleges(No.08KJA530001)
文摘Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms were of Brunauer type I and well correlated with Langmuir-Freundlich model. After sodium ions exchange, the adsorption amounts of three adsorbates increased, while the increase magnitude of CO2 adsorption capacity was much higher than that of CH4 and N2. The selectivities of CO2 over CH4 and CO2 over N2 enhanced after sodium exchange. Also, the initial heat of adsorption data implied a stronger interaction of CO2 molecules with Na+ ions in Naβ . These results can be attributed to the larger electrostatic interaction of CO2 with extraframework cations in zeolites. However, Naβ showed a decrease in the selectivity of CH4 over N2, which can be ascribed to the moderate affinity of N2 with Naβ. The variation of isosteric heats of adsorption as a function of loading indicates that the adsorption of CO2 in Naβ presents an energetically heterogeneous profile. On the contrary, the adsorption of CH4 was found to be essentially homogeneous, which suggests the dispersion interaction between CH4 and lattice oxygen atoms, and such interaction does not depend on the exchangeable cations of zeolite.
文摘用相同摩尔浓度的硝酸铵,柠檬酸以及柠檬酸铵溶液对Naβ沸石进行改性处理得到Hβ沸石;采用XRD、XRF、FT-IR、27Al MAS NMR和29Si MAS NMR等表征手段进行分析。结果表明,采用含羟基的柠檬酸或柠檬酸铵对Naβ沸石进行改性处理,不但可以提高样品结晶度还可以有效限制骨架铝的脱除;经柠檬酸或柠檬酸铵改性可以使Naβ中的Al(S4R,SiteA)转化成Al(S6R,SiteB),而硝酸铵改性的Naβ沸石中只发现一种骨架四面体;还发现硝酸铵和柠檬酸铵改性Naβ沸石后,少量的骨架铝转化为非骨架铝并存在于孔道内,而经过柠檬酸改性后,这部分非骨架铝被带出孔道。
文摘用相同物质的量浓度的硝酸铵、柠檬酸以及柠檬酸铵溶液对Naβ沸石进行改性处理得到Hβ沸石;采用XRD、XRF、FT-IR、27Al MAS NMR和29Si MAS NMR等表征手段进行分析。结果表明,采用含羟基的柠檬酸或柠檬酸铵对Naβ沸石进行改性处理,不但可以提高样品结晶度还可以有效限制骨架铝的脱除;经柠檬酸或柠檬酸铵改性可以使Naβ中的Al(S4R,SiteA)转化成Al(S6R,SiteB),而硝酸铵改性的Naβ沸石中只发现一种骨架四面体;还发现硝酸铵和柠檬酸铵改性Naβ沸石后,少量的骨架铝转化为非骨架铝并存在于孔道内,而经过柠檬酸改性后,这部分非骨架铝被带出孔道。
文摘 1.IntroductionDunn and Farrington[1]found that theNa ion in Naβ″-alumina single crystal canbe exchanged completely or partially withGd;,Nd;,Eu;,Yb;,Sm;,Tb;,Dy;,Bi;and Pr;ions,but no reports havebeen published about the ion exchange reac-tion between La3+ and Naβ″-alumina.If anion exchanged polycrystalline β″-alumina isavailable and its ionic conductivity is highenough to be applied as a solid electrolyte inthe galvanic cell,it can be used in various