铁有机骨架材料对偶氮型阴离子染料的吸附
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摘要
金属有机骨架材料由于结构可调、可选择性吸附和可再生性等优点成为处理染料废水的新型材料。以常温下合成的铁有机骨架材料作为吸附剂,探索铁有机骨架材料对具有相似结构的阴离子染料吸附性能的影响。结果表明:在酸性条件下,铁有机骨架材料对染料的脱色率更高;并且材料对阴离子染料的吸附量随着染料初始浓度的增大而增大。Langmuir恒温吸附模型可以很好地描述吸附过程,计算得到的饱和吸附量随着染料分子截面积的增加而减小。对吸附机理进行探讨发现:Fe-BDC的电荷中心与阴离子染料之间的静电引力是吸附的主要作用力,染料分子中羟基、氨基等含有孤对电子的官能团与Fe-BDC中铁原子的相互作用也是吸附的重要作用力。
Metal organic framework materials have been regarded as new absorbents for treating dye wastewater due to their controllable structure, selective adsorption and recyclable capacity. The iron-organic framework synthesized at room temperature was used as adsorbents to explore its effect on adsorption properties of anionic dyes with similar structure. The experimental findings showed that the iron organic framework had higher de-colorization for these dyes under acid condition.And the adsorption capacity increased with increase of the initial dye concentration. The adsorption process was well fitted with the Langmuir isotherms. The maximum adsorption capacity calculated from isotherm decreased with the increase of cross-sectional area of dye molecules. The electrostatic interaction between the charge center of Fe-BDC and the anionic dye was considered to be the main mechanism of adsorption. Finally,it was found that the interaction also existed between the hydroxyl,amidogen and functional groups with lone pair electrons in dye molecules and the iron atom in Fe-BDC. It also promoted the adsorption process significantly.
Metal organic framework materials have been regarded as new absorbents for treating dye wastewater due to their controllable structure, selective adsorption and recyclable capacity. The iron-organic framework synthesized at room temperature was used as adsorbents to explore its effect on adsorption properties of anionic dyes with similar structure. The experimental findings showed that the iron organic framework had higher de-colorization for these dyes under acid condition.And the adsorption capacity increased with increase of the initial dye concentration. The adsorption process was well fitted with the Langmuir isotherms. The maximum adsorption capacity calculated from isotherm decreased with the increase of cross-sectional area of dye molecules. The electrostatic interaction between the charge center of Fe-BDC and the anionic dye was considered to be the main mechanism of adsorption. Finally,it was found that the interaction also existed between the hydroxyl,amidogen and functional groups with lone pair electrons in dye molecules and the iron atom in Fe-BDC. It also promoted the adsorption process significantly.
引文
[1]任南琪,周显娇,郭婉茜,等.染料废水处理技术研究进展[J].化工学报,2013,64(1):84-94.
[2] Danwittayakul S,Jaisai M,Dutta J. Efficient solar photocatalytic degradation of textile wastewater using ZnO/ZTO composites[J].Applied Catalysis B:Environmental,2015,163:1-8.
[3] Rong H,Gao B,Li R,et al. Effect of dose methods of a synthetic organic polymer and PFC on floc properties in dyeing wastewater coagulation process[J]. Chemical Engineering Journal,2014,243(4):169-175.
[4]史欢欢,赵建海,李海燕,等.活性炭负载二氧化锰的制备及其对罗丹明B吸附效能[J].环境工程,2017,35(9):58-63.
[5] Sun D S,Zhang X D,Wu Y D,et al. Adsorption of anionic dyes from aqueous solution on fly ash[J]. Journal of Hazardous Materials,2010,181(1):335-342.
[6] Visa M,Andronic L,Lucaci D,et al. Concurrent dyes adsorption and photo-degradation on fly ash based substrates[J]. Adsorptionjournal of the International Adsorption Society,2011,17(1):101-108.
[7]孙德帅,郑强强,张晓东,等.粉煤灰对阴离子水溶性混合染料的吸附动力学[J].环境科学,2014,35(7):2590-2595.
[8] Wang J,Xue C,Wu Z,et al. Hollow micro-mesoporous carbon polyhedra produced by selective removal of skeletal scaffolds[J].Carbon,2012,50(7):2546-2555.
[9]姜爽,吕琳琳,郭宏伟.榛子壳对亚甲基蓝吸附性能的研究[J].天然产物研究与开发,2017(1):110-113.
[10]黄晓东,李茜,黄雅丽.榴莲壳粉-聚偏氟乙烯复合膜对次甲基蓝吸附的研究[J].环境工程,2018,36(2):54-59.
[11] Luo F,Yan C,Dang L,et al. UTSA-74:a MOF-74 isomer with two accessible binding sites per metal center for highly selective gas separation[J]. Journal of the American Chemical Society,2016,138(17):5678-5684.
[12] Xiang Z,Peng X,Cheng X,et al. CNT@Cu3(BTC)2and metalorganic frameworks for separation of CO2/CH4mixture[J]. Journal of Physical Chemistry C,2014,115(40):19864-19871.
[13] Yu J,Xie L H,Li J R,et al. CO2capture and separations using MOFs:computational and experimental studies[J]. Chemical Reviews,2017,117(14):9674-9754.
[14] Sun D,Lin Y,Li Z. Visible-light-assisted aerobic photocatalytic oxidation of amines to imines over NH2-MIL-125(Ti)[J]. Applied Catalysis B Environmental,2015,164(164):428-432.
[15] Chen Y F,Tan L L,Liu J M,et al. Calix[4]arene based dyesensitized Pt@Ui O-66-NH2,metal-organic framework for efficient visible-light photocatalytic hydrogen production[J]. Applied Catalysis B:Environmental,2017,206:426-433.
[16]孙德帅,刘亚丽,张晓东,等.铁有机骨架材料的快速合成及对阴离子染料的吸附性能[J].环境科学,2016,37(3):1016-1022.
[17] Haque E,Lee J E,Jang I T,et al. Adsorptive removal of methyl orange from aqueous solution with metal-organic frameworks,porous chromium-benzenedicarboxylates[J]. Journal of Hazardous Materials,2010,181(1/3):535-542.
[18] Haque E,Jun J W,Jhung S H. Adsorptive removal of methyl orange and methylene blue from aqueous solution with a metalorganic framework material,iron terephthalate(MOF-235)[J].Journal of Hazardous Materials,2011,185(1):507-511.
[19] Haque E,Lo V,Minett A I,et al. Dichotomous adsorption behaviour of dyes on an amino-functionalised metal-organic framework, amino-MIL-101(Al)[J]. Journal of Materials Chemistry A,2013,2(1):193-203.
[20] Fan Y H,Zhang S W,Qin S B,et al. An enhanced adsorption of organic dyes onto NH2functionalization titanium-based metalorganic frameworks and the mechanism investigation[J].Microporous&Mesoporous Materials,2018,263:120-127.
[21] Huo S H,Yan X P. Metal-organic framework MIL-100(Fe)for the adsorption of malachite green from aqueous solution[J]. Journal of Materials Chemistry,2012,22(15):7449-7455.
[22] Lin S,Song Z,Che G,et al. Adsorption behavior of metal-organic frameworks for methylene blue from aqueous solution[J].Microporous&Mesoporous Materials,2014,193(2):27-34.
[23] Oveisi M,Asli M A,Mahmoodi N M. MIL-Ti metal-organic frameworks(MOFs)nanomaterials as superior adsorbents:synthesis and ultrasound-aided dye adsorption from multicomponent wastewater systems[J]. Journal of Hazardous Materials,2018,347:123-140.
[24] Qin Q,Ma J,Liu K. Adsorption of anionic dyes on ammoniumfunctionalized MCM-41[J]. Journal of Hazardous Materials,2009,162(1):133-139.
[25] Yamada T,Shiraishi K,Kitagawa H,et al. Applicability of MIL-101(Fe)as a cathode of lithium ion batteries[J]. Chemical Communications,2017,53(58):8215-8218.
[26] Sudik A C,CotéA P,Yaghi O M. Metal-organic frameworks based on trigonal prismatic building blocks and the new “acs”topology[J]. Inorganic Chemistry,2005,44(9):2998-3000.
[27]孙德帅,杨振楠,郭庆杰.粉煤灰对染料的吸附脱色[J].非金属矿,2009,32(2):79-81.
[28] Dedryvère R, Maccario M, Croguennec L, et al. X-Ray photoelectron spectroscopy investigations of carbon-coated Lix Fe PO4materials[J]. Chemistry of Materials,2008,20(22):7164-7170.
[29]朱晨明,王保登,张中正,等.金属-有机骨架复合材料的制备及其二氧化碳吸附性能[J].化工进展,2016,35(9):2875-2884.
[2] Danwittayakul S,Jaisai M,Dutta J. Efficient solar photocatalytic degradation of textile wastewater using ZnO/ZTO composites[J].Applied Catalysis B:Environmental,2015,163:1-8.
[3] Rong H,Gao B,Li R,et al. Effect of dose methods of a synthetic organic polymer and PFC on floc properties in dyeing wastewater coagulation process[J]. Chemical Engineering Journal,2014,243(4):169-175.
[4]史欢欢,赵建海,李海燕,等.活性炭负载二氧化锰的制备及其对罗丹明B吸附效能[J].环境工程,2017,35(9):58-63.
[5] Sun D S,Zhang X D,Wu Y D,et al. Adsorption of anionic dyes from aqueous solution on fly ash[J]. Journal of Hazardous Materials,2010,181(1):335-342.
[6] Visa M,Andronic L,Lucaci D,et al. Concurrent dyes adsorption and photo-degradation on fly ash based substrates[J]. Adsorptionjournal of the International Adsorption Society,2011,17(1):101-108.
[7]孙德帅,郑强强,张晓东,等.粉煤灰对阴离子水溶性混合染料的吸附动力学[J].环境科学,2014,35(7):2590-2595.
[8] Wang J,Xue C,Wu Z,et al. Hollow micro-mesoporous carbon polyhedra produced by selective removal of skeletal scaffolds[J].Carbon,2012,50(7):2546-2555.
[9]姜爽,吕琳琳,郭宏伟.榛子壳对亚甲基蓝吸附性能的研究[J].天然产物研究与开发,2017(1):110-113.
[10]黄晓东,李茜,黄雅丽.榴莲壳粉-聚偏氟乙烯复合膜对次甲基蓝吸附的研究[J].环境工程,2018,36(2):54-59.
[11] Luo F,Yan C,Dang L,et al. UTSA-74:a MOF-74 isomer with two accessible binding sites per metal center for highly selective gas separation[J]. Journal of the American Chemical Society,2016,138(17):5678-5684.
[12] Xiang Z,Peng X,Cheng X,et al. CNT@Cu3(BTC)2and metalorganic frameworks for separation of CO2/CH4mixture[J]. Journal of Physical Chemistry C,2014,115(40):19864-19871.
[13] Yu J,Xie L H,Li J R,et al. CO2capture and separations using MOFs:computational and experimental studies[J]. Chemical Reviews,2017,117(14):9674-9754.
[14] Sun D,Lin Y,Li Z. Visible-light-assisted aerobic photocatalytic oxidation of amines to imines over NH2-MIL-125(Ti)[J]. Applied Catalysis B Environmental,2015,164(164):428-432.
[15] Chen Y F,Tan L L,Liu J M,et al. Calix[4]arene based dyesensitized Pt@Ui O-66-NH2,metal-organic framework for efficient visible-light photocatalytic hydrogen production[J]. Applied Catalysis B:Environmental,2017,206:426-433.
[16]孙德帅,刘亚丽,张晓东,等.铁有机骨架材料的快速合成及对阴离子染料的吸附性能[J].环境科学,2016,37(3):1016-1022.
[17] Haque E,Lee J E,Jang I T,et al. Adsorptive removal of methyl orange from aqueous solution with metal-organic frameworks,porous chromium-benzenedicarboxylates[J]. Journal of Hazardous Materials,2010,181(1/3):535-542.
[18] Haque E,Jun J W,Jhung S H. Adsorptive removal of methyl orange and methylene blue from aqueous solution with a metalorganic framework material,iron terephthalate(MOF-235)[J].Journal of Hazardous Materials,2011,185(1):507-511.
[19] Haque E,Lo V,Minett A I,et al. Dichotomous adsorption behaviour of dyes on an amino-functionalised metal-organic framework, amino-MIL-101(Al)[J]. Journal of Materials Chemistry A,2013,2(1):193-203.
[20] Fan Y H,Zhang S W,Qin S B,et al. An enhanced adsorption of organic dyes onto NH2functionalization titanium-based metalorganic frameworks and the mechanism investigation[J].Microporous&Mesoporous Materials,2018,263:120-127.
[21] Huo S H,Yan X P. Metal-organic framework MIL-100(Fe)for the adsorption of malachite green from aqueous solution[J]. Journal of Materials Chemistry,2012,22(15):7449-7455.
[22] Lin S,Song Z,Che G,et al. Adsorption behavior of metal-organic frameworks for methylene blue from aqueous solution[J].Microporous&Mesoporous Materials,2014,193(2):27-34.
[23] Oveisi M,Asli M A,Mahmoodi N M. MIL-Ti metal-organic frameworks(MOFs)nanomaterials as superior adsorbents:synthesis and ultrasound-aided dye adsorption from multicomponent wastewater systems[J]. Journal of Hazardous Materials,2018,347:123-140.
[24] Qin Q,Ma J,Liu K. Adsorption of anionic dyes on ammoniumfunctionalized MCM-41[J]. Journal of Hazardous Materials,2009,162(1):133-139.
[25] Yamada T,Shiraishi K,Kitagawa H,et al. Applicability of MIL-101(Fe)as a cathode of lithium ion batteries[J]. Chemical Communications,2017,53(58):8215-8218.
[26] Sudik A C,CotéA P,Yaghi O M. Metal-organic frameworks based on trigonal prismatic building blocks and the new “acs”topology[J]. Inorganic Chemistry,2005,44(9):2998-3000.
[27]孙德帅,杨振楠,郭庆杰.粉煤灰对染料的吸附脱色[J].非金属矿,2009,32(2):79-81.
[28] Dedryvère R, Maccario M, Croguennec L, et al. X-Ray photoelectron spectroscopy investigations of carbon-coated Lix Fe PO4materials[J]. Chemistry of Materials,2008,20(22):7164-7170.
[29]朱晨明,王保登,张中正,等.金属-有机骨架复合材料的制备及其二氧化碳吸附性能[J].化工进展,2016,35(9):2875-2884.