磁性Ca/Al水滑石对活性艳红X-3B吸附的响应曲面法优化
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摘要
采用超声辅助法以超顺磁性铁氧体材料对制备的Ca/Al水滑石进行复合改性合成磁性Ca/Al水滑石,并研究其对活性艳红X-3B模拟染料废水的吸附性能。考察了磁性Ca/Al水滑石吸附剂剂量、吸附时间和初始pH值对活性艳红X-3B染料废水脱色效果的影响,采用Design-Expert软件对吸附条件进行了Box-Behnken响应曲面法优化。实验结果表明:当吸附剂剂量为7.6g/L,吸附时间为32.3min,初始pH值为6.9时,该材料对活性艳红X-3B染料的理论最大脱色率为94.2%.由于材料自身的磁性特性,吸附后的悬浊液在外加磁场的作用下,能够实现磁性水滑石的快速回收。同时,对回收再生磁性Ca/Al水滑石的吸附性能进行了研究,发现在吸附-解吸3次循环后仍然有很好的脱色效果,表明该磁性Ca/Al水滑石是一种极具潜力的新型染料吸附剂。
Ultrasound-assisted method was used to synthesize magnetic Ca/Al layered double hydroxides,and decoloration efficiency of reactive brilliant red X-3 Bsimulated dye wastewater was studied.The effect of adsorbent dosage,adsorption time,and initial pH was investigated on the decolorization efficiency of reactive brilliant red X-3 Bdye wastewater,and the Box-Behnken response surface methodology(RSM)was used to optimize the adsorption conditions.The experimental results show that when the adsorbent dosage is 7.6 g/L,the adsorption time is 32.3 min and the initial pH is 6.9,the theoretical maximum decolorization rate of the reactive brilliant red X-3 Bis 94.2%.Owing to the magnetic characteristics of the material,after adsorption,magnetic Ca/Al layered double hydroxides can be quickly recovered from the suspension in an externed magnetic field.Meanwhile,the adsorption property of regenerated magnetic Ca/Al layered double hydroxides was studied.After 3 adsorption-desorption cycles the matenial still had a good decoloration efficiency,indicating that the magnetic Ca/Al hydrotalcite is a potential new type of dye adsorbent.
Ultrasound-assisted method was used to synthesize magnetic Ca/Al layered double hydroxides,and decoloration efficiency of reactive brilliant red X-3 Bsimulated dye wastewater was studied.The effect of adsorbent dosage,adsorption time,and initial pH was investigated on the decolorization efficiency of reactive brilliant red X-3 Bdye wastewater,and the Box-Behnken response surface methodology(RSM)was used to optimize the adsorption conditions.The experimental results show that when the adsorbent dosage is 7.6 g/L,the adsorption time is 32.3 min and the initial pH is 6.9,the theoretical maximum decolorization rate of the reactive brilliant red X-3 Bis 94.2%.Owing to the magnetic characteristics of the material,after adsorption,magnetic Ca/Al layered double hydroxides can be quickly recovered from the suspension in an externed magnetic field.Meanwhile,the adsorption property of regenerated magnetic Ca/Al layered double hydroxides was studied.After 3 adsorption-desorption cycles the matenial still had a good decoloration efficiency,indicating that the magnetic Ca/Al hydrotalcite is a potential new type of dye adsorbent.
引文
[1]ARMAGAN B,TURAN M,ELIK M S.Equilibrium studies on the adsorption of reactive azo dyes into zeolite[J].Desalination,2004,170(1):33-39.
[2]RACHE M L,GARCIA A R,ZEA H R,et al.Azo-dye orange II degradation by the heterogeneous Fenton-like process using a zeolite Y-Fe catalyst-Kinetics with a model based on the Fermi's equation[J].Applied Catalysis B Environmental,2014,146:192-200.
[3]MAYER R L.Aromatic amines and azo-dyes in allergy and cancer[J].Journal of Investigative Dermatology,1948,10(5):389-396.
[4]SOLISABBBA M.Microbial decolouration of azo dyes:A review[J].Process Biochemistry,2012,47(12):1723-1748.
[5]丁绍兰,李郑坤,王睿.染料废水处理技术综述[J].水资源保护,2010,26(3):73-78.DING S L,LI Z K,WANG R.Summary of treatment of dyestuff wastewater[J].Water Resources Protection,2010,26(3):73-78.
[6]CRINI G.Non-conventional low-cost adsorbents for dye removal:a review[J].Bioresource technology,2006,97(9):1061-1085.
[7]陆朝阳,沈莉莉,张全兴.吸附法处理染料废水的工艺及其机理研究进展[J].工业水处理,2004,24(3):12-16.LU Z Y,SHEN L L,ZHANG Q X.Research development of technics and mechanism of dye wastewater treatment by adsorption[J].Industrial Water Treatment,2004,24(3):12-16.
[8]TYAGI S B,KHARKWAL A,NITU,et al.Synthesis and characterization of layered double hydroxides containing optically active transition metal ion[J].Solid State Sciences,2017,63:93-102.
[9]GOH K H,LIM T T,DONG Z.Application of layered double hydroxides for removal of oxyanions:a review[J].Water research,2008,42(6/7):1343-1368.
[10]ZHANG C,YANG S,CHEN H,et al.Adsorption behavior and mechanism of reactive brilliant red X-3Bin aqueous solution over three kinds of hydrotalcite-like LDHs[J].Applied Surface Science,2014,301(10):329-337.
[11]NGOMSIK A F,BEE A,DRAYE M,et al.Magnetic nano-and microparticles for metal removal and environmental applications:a review[J].Comptes Rendus Chimie,2005,8(6/7):963-970.
[12]SHAN R R,YAN L G,YANG K,et al.Magnetic Fe3O4/MgAl-LDH composite for effective removal of three red dyes from aqueous solution[J].Chemical Engineering Journal,2014,252:38-46.
[13]ZHANG X,JI L,WANG J,et al.Removal of uranium(VI)from aqueous solutions by magnetic Mg-Al layered double hydroxide intercalated with citrate:Kinetic and thermodynamic investigation[J].Colloids&Surfaces A Physicochemical&Engineering Aspects,2012,414(46):220-227.
[14]李松南.磁性水滑石及其改性材料对六价铬及铜离子吸附性能的研究[D].哈尔滨:哈尔滨工程大学,2009.LI S N.Adsorption of hexavalent chromium and copper ions by magnetic layered double hydroxides[D].Harbin:Harbin Engineering University,2009.
[15]陈爱燕,程翔,黄新瑞,等.Zn-Al类水滑石磷吸附剂的制备及其吸附性能[J].化工学报,2008,59(9):2270-2275.CHEN A Y,CHENG X,HUANG X R,et al.Synthesis of Zn-Al hydrotalcite-like compounds as phosphate adsorbent and its adsorption capacity[J].CIESC Journal,2008,59(9):2270-2275.
[16]常青,江国栋,胡梦璇,等.石墨烯基磁性复合材料吸附水中亚甲基蓝的研究[J].环境科学,2014,35(5):1804-1809.CHANG Q,JIANG G D,HU M X,et al.Adsorption of methylene blue from aqueous solution onto magnetic Fe3O4/graphene oxide nanoparticles[J].Environment Science,2014,35(5):1804-1809.
[17]AUXILIO A R,ANDREWS P C,JUNK P C,et al.Adsorption and intercalation of acid blue 9on Mg-Al layered double hydroxides of variable metal composition[J].Polyhedron,2007,26(14):3479-3490.
[18]FERREIRA S L C,BRUNS R E,FERREIRA H S,et al.Box-behnken design:an alternative for the optimization of analytical methods[J].Analytica Chimica Acta,2007,597(2):179-186.
[19]BEZERRA M A,SANTELLI R E,OLIVEIRA E P,et al.Response surface methodology(RSM)as a tool for optimization in analytical chemistry[J].Talanta,2008,76(5):965-977.
[20]段绍君,孙玉柱,宋兴福,等.响应曲面法优化碳酸锂反应结晶工艺[J].化工学报,2017,68(11):4169-4177.DUAN S J,SUN Y Z,SONG X F,et al.Optimization of reactive-crystallization process of lithium carbonate based on response surface methodology[J].CIESC Journal,2017,68(11):4169-4177.
[21]邢奕,王志强,洪晨,等.基于RSM模型对污泥联合调理的参数优化[J].中国环境科学,2014,34(11):2866-2873.XING Y,WANG Z Q,HONG C,et al.Parameter optimization of sludge co-conditioning based on RSM model[J].China Environmental Science,2014,34(11):2866-2873.
[22]张晖,HUANG C P.响应面法分析卫生填埋渗滤液的Fenton处理过程[J].环境科学,2003,24(4):142-145.ZHANG H,HUANG C P.Evaluation of fenton process for the treatment of sanitary landfill leachate with response surface methodology[J].Environment Science,2003,24(4):142-145.
[23]牛向楠,赵毅,朱洪涛.Mg-Al水滑石对偶氮染料活性艳红X-3B的脱色性能研究[J].环境工程学报,2011,5(12):2813-2819.NIU X N,ZHAO Y,ZHU H T.Study on decoloration of wastewater containing active red X-3Bby Mg-Al layered double hydroxides[J].Chinese Journal of Environmental Engineering,2011,5(12):2813-2819.
[24]于洋,岳秀萍,刘吉明,等.Mg/Al/Fe型类水滑石焙烧产物吸附去除水中硫酸根离子[J].环境工程学报,2013,7(8):3079-3084.YU Y,YUE X P,LIU J M,et al.Removal of sulfate ions from aqueous solution via adsorption on calcined Mg/Al/Fe hydrotalcite-like compounds[J].Chinese Journal of Environmental Engineering,2013,7(8):3079-3084.
[25]李松南.以蛋壳为原料制备多种吸附材料及其铀吸附性能研究[D].哈尔滨:哈尔滨工程大学,2013.LI S N.Study on the conversion of eggshells into different adsorbent materials and their adsorption properties of uranium[D].Harbin:Harbin Engineering University,2013.
[26]DHODAPKAR R,RAO N N,PANDE S P,et al.Adsorption of cationic dyes on jalshakti,super absorbent polymer and photocatalytic regeneration of the adsorbent[J].Reactive&Functional Polymers,2007,67(6):540-548.
[27]EXTREMERA R,PAVLOVIC I,PEREZ M R,et al.Removal of acid orange 10by calcined Mg/Al layered double hydroxides from water and recovery of the adsorbed dye[J].Chemical Engineering Journal,2012,213(12):392-400.
[2]RACHE M L,GARCIA A R,ZEA H R,et al.Azo-dye orange II degradation by the heterogeneous Fenton-like process using a zeolite Y-Fe catalyst-Kinetics with a model based on the Fermi's equation[J].Applied Catalysis B Environmental,2014,146:192-200.
[3]MAYER R L.Aromatic amines and azo-dyes in allergy and cancer[J].Journal of Investigative Dermatology,1948,10(5):389-396.
[4]SOLISABBBA M.Microbial decolouration of azo dyes:A review[J].Process Biochemistry,2012,47(12):1723-1748.
[5]丁绍兰,李郑坤,王睿.染料废水处理技术综述[J].水资源保护,2010,26(3):73-78.DING S L,LI Z K,WANG R.Summary of treatment of dyestuff wastewater[J].Water Resources Protection,2010,26(3):73-78.
[6]CRINI G.Non-conventional low-cost adsorbents for dye removal:a review[J].Bioresource technology,2006,97(9):1061-1085.
[7]陆朝阳,沈莉莉,张全兴.吸附法处理染料废水的工艺及其机理研究进展[J].工业水处理,2004,24(3):12-16.LU Z Y,SHEN L L,ZHANG Q X.Research development of technics and mechanism of dye wastewater treatment by adsorption[J].Industrial Water Treatment,2004,24(3):12-16.
[8]TYAGI S B,KHARKWAL A,NITU,et al.Synthesis and characterization of layered double hydroxides containing optically active transition metal ion[J].Solid State Sciences,2017,63:93-102.
[9]GOH K H,LIM T T,DONG Z.Application of layered double hydroxides for removal of oxyanions:a review[J].Water research,2008,42(6/7):1343-1368.
[10]ZHANG C,YANG S,CHEN H,et al.Adsorption behavior and mechanism of reactive brilliant red X-3Bin aqueous solution over three kinds of hydrotalcite-like LDHs[J].Applied Surface Science,2014,301(10):329-337.
[11]NGOMSIK A F,BEE A,DRAYE M,et al.Magnetic nano-and microparticles for metal removal and environmental applications:a review[J].Comptes Rendus Chimie,2005,8(6/7):963-970.
[12]SHAN R R,YAN L G,YANG K,et al.Magnetic Fe3O4/MgAl-LDH composite for effective removal of three red dyes from aqueous solution[J].Chemical Engineering Journal,2014,252:38-46.
[13]ZHANG X,JI L,WANG J,et al.Removal of uranium(VI)from aqueous solutions by magnetic Mg-Al layered double hydroxide intercalated with citrate:Kinetic and thermodynamic investigation[J].Colloids&Surfaces A Physicochemical&Engineering Aspects,2012,414(46):220-227.
[14]李松南.磁性水滑石及其改性材料对六价铬及铜离子吸附性能的研究[D].哈尔滨:哈尔滨工程大学,2009.LI S N.Adsorption of hexavalent chromium and copper ions by magnetic layered double hydroxides[D].Harbin:Harbin Engineering University,2009.
[15]陈爱燕,程翔,黄新瑞,等.Zn-Al类水滑石磷吸附剂的制备及其吸附性能[J].化工学报,2008,59(9):2270-2275.CHEN A Y,CHENG X,HUANG X R,et al.Synthesis of Zn-Al hydrotalcite-like compounds as phosphate adsorbent and its adsorption capacity[J].CIESC Journal,2008,59(9):2270-2275.
[16]常青,江国栋,胡梦璇,等.石墨烯基磁性复合材料吸附水中亚甲基蓝的研究[J].环境科学,2014,35(5):1804-1809.CHANG Q,JIANG G D,HU M X,et al.Adsorption of methylene blue from aqueous solution onto magnetic Fe3O4/graphene oxide nanoparticles[J].Environment Science,2014,35(5):1804-1809.
[17]AUXILIO A R,ANDREWS P C,JUNK P C,et al.Adsorption and intercalation of acid blue 9on Mg-Al layered double hydroxides of variable metal composition[J].Polyhedron,2007,26(14):3479-3490.
[18]FERREIRA S L C,BRUNS R E,FERREIRA H S,et al.Box-behnken design:an alternative for the optimization of analytical methods[J].Analytica Chimica Acta,2007,597(2):179-186.
[19]BEZERRA M A,SANTELLI R E,OLIVEIRA E P,et al.Response surface methodology(RSM)as a tool for optimization in analytical chemistry[J].Talanta,2008,76(5):965-977.
[20]段绍君,孙玉柱,宋兴福,等.响应曲面法优化碳酸锂反应结晶工艺[J].化工学报,2017,68(11):4169-4177.DUAN S J,SUN Y Z,SONG X F,et al.Optimization of reactive-crystallization process of lithium carbonate based on response surface methodology[J].CIESC Journal,2017,68(11):4169-4177.
[21]邢奕,王志强,洪晨,等.基于RSM模型对污泥联合调理的参数优化[J].中国环境科学,2014,34(11):2866-2873.XING Y,WANG Z Q,HONG C,et al.Parameter optimization of sludge co-conditioning based on RSM model[J].China Environmental Science,2014,34(11):2866-2873.
[22]张晖,HUANG C P.响应面法分析卫生填埋渗滤液的Fenton处理过程[J].环境科学,2003,24(4):142-145.ZHANG H,HUANG C P.Evaluation of fenton process for the treatment of sanitary landfill leachate with response surface methodology[J].Environment Science,2003,24(4):142-145.
[23]牛向楠,赵毅,朱洪涛.Mg-Al水滑石对偶氮染料活性艳红X-3B的脱色性能研究[J].环境工程学报,2011,5(12):2813-2819.NIU X N,ZHAO Y,ZHU H T.Study on decoloration of wastewater containing active red X-3Bby Mg-Al layered double hydroxides[J].Chinese Journal of Environmental Engineering,2011,5(12):2813-2819.
[24]于洋,岳秀萍,刘吉明,等.Mg/Al/Fe型类水滑石焙烧产物吸附去除水中硫酸根离子[J].环境工程学报,2013,7(8):3079-3084.YU Y,YUE X P,LIU J M,et al.Removal of sulfate ions from aqueous solution via adsorption on calcined Mg/Al/Fe hydrotalcite-like compounds[J].Chinese Journal of Environmental Engineering,2013,7(8):3079-3084.
[25]李松南.以蛋壳为原料制备多种吸附材料及其铀吸附性能研究[D].哈尔滨:哈尔滨工程大学,2013.LI S N.Study on the conversion of eggshells into different adsorbent materials and their adsorption properties of uranium[D].Harbin:Harbin Engineering University,2013.
[26]DHODAPKAR R,RAO N N,PANDE S P,et al.Adsorption of cationic dyes on jalshakti,super absorbent polymer and photocatalytic regeneration of the adsorbent[J].Reactive&Functional Polymers,2007,67(6):540-548.
[27]EXTREMERA R,PAVLOVIC I,PEREZ M R,et al.Removal of acid orange 10by calcined Mg/Al layered double hydroxides from water and recovery of the adsorbed dye[J].Chemical Engineering Journal,2012,213(12):392-400.