以十六烷基三甲基溴化铵(CTAB)表面活性剂和钛酸四丁酯分别为造孔模板和钛源,通过超声辅助溶剂挥发自组装技术制备有序介孔氧化钛(ordered mesoporous Ti O2,OMPT)及其活性炭负载体(ordered mesoporous Ti O2/AC,OMPTA).为探讨OMPTA结...以十六烷基三甲基溴化铵(CTAB)表面活性剂和钛酸四丁酯分别为造孔模板和钛源,通过超声辅助溶剂挥发自组装技术制备有序介孔氧化钛(ordered mesoporous Ti O2,OMPT)及其活性炭负载体(ordered mesoporous Ti O2/AC,OMPTA).为探讨OMPTA结构与性能之间的关系,采用超声辅助溶胶-凝胶技术合成了无孔氧化钛/活性炭(nonporous Ti O2/AC,NPTA)负载体,利用热重-差热(TG-DTA)、X射线衍射(XRD)、氮气吸附-解吸、透射电子显微镜(TEM)和紫外漫反射(DRS)等手段对制备材料结构进行表征.以酸性红B(acid red B,ARB)的光催化降解为探针实验,评价OMPTA的光催化性能和使用寿命,提出了孔-孔协同光催化扩增机制,并探讨了催化条件(染料浓度、催化剂浓度和溶液p H)对协同扩增效果的影响.结果表明:相对于纯OMPT,OMPTA具有晶粒生长的高活化能、较小的粒径尺寸和对有序介孔结构的高热稳定性,这归功于活性炭的吸附力和非晶相层对晶粒生长的阻碍作用.由于孔-孔协同光催化扩增效应,导致OMPTA在NPTA、OMPT-AC、OMPT、P25和NPT中具有更高的催化活性.热处理温度强烈影响OMPTA的光催化活性,其中OMPTA-500具有最高的光催化活性,这归功于其具备完善的结晶性、相对高浓度的羟基和Ti3+离子.同时,OMPTA-500在重复使用过程中也具有很高的光催化性能.当使用OMPTA-500为催化剂对ARB降解时,最佳的催化条件为催化剂浓度1 g/L,ARB浓度15 mg/L,p H 5.展开更多
To study the mechanism by which activated carbon is modified by HNO3 and Mn(NO3)2,the pore texture and surface chemical characteristics of carbon materials in coconut husk activated carbon(AC)were examined via scannin...To study the mechanism by which activated carbon is modified by HNO3 and Mn(NO3)2,the pore texture and surface chemical characteristics of carbon materials in coconut husk activated carbon(AC)were examined via scanning electron microscopy(SEM),Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),and X-ray photoelectron spectroscopy(XPS).After being modified by HNO3,the millipore character of AC became deformed,and the character of the adjacent pores remained consolidated.The surface manganites of Mn/AC-1 presented as block and reticular fiber structures,Mn/AC-2's surface manganites presented as petty mammock crystals,and Mn/AC-3's surface manganites were observed as gauze nanosheets that interlace to fill in the pore canal.Nitric acid modification was shown to enlarge surface pores but decrease the specific surface area of AC.Mn loading can be used to construct a new pore structure that,in turn,increased the total specific surface area as well as the specific surface area and the volume of the millipores.Mn/AC-2's pore structure was optimized at a calcination temperature of 500℃and a loading quantity of 5%.The ash content of AC was considerably reduced after modified by HNO3.The active materials for Mn/AC-1 mainly consisted of Mn3O4,with a few Mn2O3 crystals,whereas Mn/AC-2's materials were mainly Mn3O4 and some MnO crystals.Mn/AC-3 was exclusively composed of Mn3O4.HNO3 activation and Mn loading modification did not considerably affect the functional group species present on the catalyst.Modification conditions using the same loading quantities and higher calcination temperatures decreased the number of O—H and N—H bonds while conversely increasing the number of CC and C—O bonds.On the contrary,the use of a higher loading quantity while maintaining the same calcination temperature increased the number of O—H and N—H bonds.A higher loading quantity is beneficial for increasing Mn^4+species.A higher calcination temperature is beneficial for increasing Mn^3+species.The results can optimize the conditions under which Mn/AC catalyst modification occurs,thus improving the physical and chemical properties of carbon-based sorbents.展开更多
Metal ion contamination of drinking water and waste water, especially with heavy metal ion such as lead, is a serious and ongoing problem. In this work, activated carbon prepared from peanut shell （PAC） was used for...Metal ion contamination of drinking water and waste water, especially with heavy metal ion such as lead, is a serious and ongoing problem. In this work, activated carbon prepared from peanut shell （PAC） was used for the removal of Pb^2＋ from aqueous solution. The impacts of the Pb25 adsorption capacities of the acid-modified carbons oxidized with HNO3 were also investigated. The surface functional groups of PAC were confirmed by Fourier transform infrared （FTIR） spectroscopy, X-ray photoelectron spectroscopy （XPS）, Boehm titration. The textural properties （surface area, total pore volume） were evaluated from the nitrogen adsorption isotherm at 77 K. The experimental results presented indicated that the adsorption data fitted better with the Langmuir adsorption model. A comparative study with a commercial granular activated carbon （GAC） showed that PAC was 10.3 times more efficient compared to GAC based on Langmuir maximum adsorption capacity. Further analysis results by the Langmuir equation showed that HNO3 [20% （by mass）] modified PAC has larger adsorption capacity of Pb^2＋ from aqueous solution （as much as 35.5 mg·g^-1）. The adsorption capacity enhancement ascribed to pore widening, increased cation-exchange capacity by oxygen groups, and the promoted hydrophilicity of the carbon surface.展开更多
The role of Nil（NO3）2 in the preparation of a magnetic activated carbon is reported in this paper. Magnetic coal-based activated carbons （MCAC） were prepared from Taixi anthracite with low ash content in the prese...The role of Nil（NO3）2 in the preparation of a magnetic activated carbon is reported in this paper. Magnetic coal-based activated carbons （MCAC） were prepared from Taixi anthracite with low ash content in the presence of Ni（NO3）2. The MCAC materials were characterized by a vibrating sample magnetometer （VSM）, X-ray diffraction （XRD）, a scanning electric microscope （SEM）, and by N2 adsorption. The cylindri- cal precursors and derived char were also subjected to thermogravimetric analysis to compare their behavior of weight losses during carbonization. The results show that MCAC has a larger surface area （1074 m21g） and a higher pore volume （0.5792 cm3/g） with enhanced mesopore ratio （by about 10~）. It also has a high saturation magnetization （1.6749 emu/g） and low coercivity （43.26 Oe）, which allows the material to be magnetically separated. The MCAC is easily magnetized because the nickel salt is con- vetted into Ni during carbonization and activation. Metallic Ni has a strong magnetism on account of electrostatic interaction. Added Ni（NO3）2 catalyzes the carbonization and activation process by accelerat- ing burn off of the carbon, which contributes to the development of mesopores and macropores in the activated carbon.展开更多
文摘以十六烷基三甲基溴化铵(CTAB)表面活性剂和钛酸四丁酯分别为造孔模板和钛源,通过超声辅助溶剂挥发自组装技术制备有序介孔氧化钛(ordered mesoporous Ti O2,OMPT)及其活性炭负载体(ordered mesoporous Ti O2/AC,OMPTA).为探讨OMPTA结构与性能之间的关系,采用超声辅助溶胶-凝胶技术合成了无孔氧化钛/活性炭(nonporous Ti O2/AC,NPTA)负载体,利用热重-差热(TG-DTA)、X射线衍射(XRD)、氮气吸附-解吸、透射电子显微镜(TEM)和紫外漫反射(DRS)等手段对制备材料结构进行表征.以酸性红B(acid red B,ARB)的光催化降解为探针实验,评价OMPTA的光催化性能和使用寿命,提出了孔-孔协同光催化扩增机制,并探讨了催化条件(染料浓度、催化剂浓度和溶液p H)对协同扩增效果的影响.结果表明:相对于纯OMPT,OMPTA具有晶粒生长的高活化能、较小的粒径尺寸和对有序介孔结构的高热稳定性,这归功于活性炭的吸附力和非晶相层对晶粒生长的阻碍作用.由于孔-孔协同光催化扩增效应,导致OMPTA在NPTA、OMPT-AC、OMPT、P25和NPT中具有更高的催化活性.热处理温度强烈影响OMPTA的光催化活性,其中OMPTA-500具有最高的光催化活性,这归功于其具备完善的结晶性、相对高浓度的羟基和Ti3+离子.同时,OMPTA-500在重复使用过程中也具有很高的光催化性能.当使用OMPTA-500为催化剂对ARB降解时,最佳的催化条件为催化剂浓度1 g/L,ARB浓度15 mg/L,p H 5.
基金The Science and Technology Plan of Yunnan Science and Technology Department(No.2019FB077,202001AT070029)the Open Fund of Key Laboratory of Ministry of Education for Metallurgical Emission Reduction and Comprehensive Utilization of Resources(No.JKF19-08)the Industrialization Cultivation Project of Scientific Research Fund of Yunnan Provincial Department of Education(No.2016CYH07).
文摘To study the mechanism by which activated carbon is modified by HNO3 and Mn(NO3)2,the pore texture and surface chemical characteristics of carbon materials in coconut husk activated carbon(AC)were examined via scanning electron microscopy(SEM),Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),and X-ray photoelectron spectroscopy(XPS).After being modified by HNO3,the millipore character of AC became deformed,and the character of the adjacent pores remained consolidated.The surface manganites of Mn/AC-1 presented as block and reticular fiber structures,Mn/AC-2's surface manganites presented as petty mammock crystals,and Mn/AC-3's surface manganites were observed as gauze nanosheets that interlace to fill in the pore canal.Nitric acid modification was shown to enlarge surface pores but decrease the specific surface area of AC.Mn loading can be used to construct a new pore structure that,in turn,increased the total specific surface area as well as the specific surface area and the volume of the millipores.Mn/AC-2's pore structure was optimized at a calcination temperature of 500℃and a loading quantity of 5%.The ash content of AC was considerably reduced after modified by HNO3.The active materials for Mn/AC-1 mainly consisted of Mn3O4,with a few Mn2O3 crystals,whereas Mn/AC-2's materials were mainly Mn3O4 and some MnO crystals.Mn/AC-3 was exclusively composed of Mn3O4.HNO3 activation and Mn loading modification did not considerably affect the functional group species present on the catalyst.Modification conditions using the same loading quantities and higher calcination temperatures decreased the number of O—H and N—H bonds while conversely increasing the number of CC and C—O bonds.On the contrary,the use of a higher loading quantity while maintaining the same calcination temperature increased the number of O—H and N—H bonds.A higher loading quantity is beneficial for increasing Mn^4+species.A higher calcination temperature is beneficial for increasing Mn^3+species.The results can optimize the conditions under which Mn/AC catalyst modification occurs,thus improving the physical and chemical properties of carbon-based sorbents.
文摘Metal ion contamination of drinking water and waste water, especially with heavy metal ion such as lead, is a serious and ongoing problem. In this work, activated carbon prepared from peanut shell （PAC） was used for the removal of Pb^2＋ from aqueous solution. The impacts of the Pb25 adsorption capacities of the acid-modified carbons oxidized with HNO3 were also investigated. The surface functional groups of PAC were confirmed by Fourier transform infrared （FTIR） spectroscopy, X-ray photoelectron spectroscopy （XPS）, Boehm titration. The textural properties （surface area, total pore volume） were evaluated from the nitrogen adsorption isotherm at 77 K. The experimental results presented indicated that the adsorption data fitted better with the Langmuir adsorption model. A comparative study with a commercial granular activated carbon （GAC） showed that PAC was 10.3 times more efficient compared to GAC based on Langmuir maximum adsorption capacity. Further analysis results by the Langmuir equation showed that HNO3 [20% （by mass）] modified PAC has larger adsorption capacity of Pb^2＋ from aqueous solution （as much as 35.5 mg·g^-1）. The adsorption capacity enhancement ascribed to pore widening, increased cation-exchange capacity by oxygen groups, and the promoted hydrophilicity of the carbon surface.
基金support by the National Natural Science Foundation of China (No. 20776150)the National Hi-Tech Research and Development Program of China(No. 2008AA05Z308)the Special Fund for Basic Scientific Research of Central Colleges (No. 2009QH15)
文摘The role of Nil（NO3）2 in the preparation of a magnetic activated carbon is reported in this paper. Magnetic coal-based activated carbons （MCAC） were prepared from Taixi anthracite with low ash content in the presence of Ni（NO3）2. The MCAC materials were characterized by a vibrating sample magnetometer （VSM）, X-ray diffraction （XRD）, a scanning electric microscope （SEM）, and by N2 adsorption. The cylindri- cal precursors and derived char were also subjected to thermogravimetric analysis to compare their behavior of weight losses during carbonization. The results show that MCAC has a larger surface area （1074 m21g） and a higher pore volume （0.5792 cm3/g） with enhanced mesopore ratio （by about 10~）. It also has a high saturation magnetization （1.6749 emu/g） and low coercivity （43.26 Oe）, which allows the material to be magnetically separated. The MCAC is easily magnetized because the nickel salt is con- vetted into Ni during carbonization and activation. Metallic Ni has a strong magnetism on account of electrostatic interaction. Added Ni（NO3）2 catalyzes the carbonization and activation process by accelerat- ing burn off of the carbon, which contributes to the development of mesopores and macropores in the activated carbon.
