改性废弃皮革吸附剂的制备及对氟的吸附性能
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摘要
将锆(Ⅳ)固化在通过乙醛酸改性的粒状废弃皮革上制备出新型氟离子吸附剂.采用SEM-EDX、XPS、FTIR等方法表征了其表面形貌及结构,研究了该吸附剂对溶液中氟离子(F-)的吸附特性并探索其吸附机理。结果表明:粒状废弃皮革与锆的最佳质量比为1∶2;对F-的吸附最佳p H=3;当p H为3,温度为25℃、F-的初始浓度为50 mg/L、吸附剂用量为0.5 g/L时,对F-的吸附量为49.72 mg/g,当吸附剂用量增加到3 g/L时,F-的去除率可达96%;该吸附剂对F-的吸附等温线符合Langmuir方程,吸附动力学可用准二级动力学模型描述,属化学吸附,F-以离子交换的形式代替-OH与吸附剂中的锆(Zr(Ⅳ))结合形成稳定的化学键,从而达到吸附水溶液中氟离子的目的。
A novel sorbent for fluoride adsorption was prepared by immobilizing Zr(Ⅳ)on glyoxylic acid(GA)-modified granular leather waste(GLW). The surface morphology and structure of adsorbent were characterized by SEM-EDX,XPS,FTIR to study characteristics of the adsorbent for fluoride and adsorption mechanism. The results indicated the optimal mass ratio of GLW/Zr(Ⅳ)was 1∶2. The optimal p H of adsorption was 3. The adsorption capacity could reach 49.72 mg/g at p H of 3,temperature of 25 ℃,initial concentration of 50 mg/L,dosage of 0.5 g/L. While the dosage increased to 3 g/L,the removal efficiency of fluoride could reach to 96%. Adsorption process could be well described by Langmuir model. The adsorption kinetic data were fitted well with pseudo-second-order model. Fluoride ion could combine with Zr(Ⅳ)on MGLW to develop a stable chemical bond by ion exchange,resulting in the removal of fluoride.
A novel sorbent for fluoride adsorption was prepared by immobilizing Zr(Ⅳ)on glyoxylic acid(GA)-modified granular leather waste(GLW). The surface morphology and structure of adsorbent were characterized by SEM-EDX,XPS,FTIR to study characteristics of the adsorbent for fluoride and adsorption mechanism. The results indicated the optimal mass ratio of GLW/Zr(Ⅳ)was 1∶2. The optimal p H of adsorption was 3. The adsorption capacity could reach 49.72 mg/g at p H of 3,temperature of 25 ℃,initial concentration of 50 mg/L,dosage of 0.5 g/L. While the dosage increased to 3 g/L,the removal efficiency of fluoride could reach to 96%. Adsorption process could be well described by Langmuir model. The adsorption kinetic data were fitted well with pseudo-second-order model. Fluoride ion could combine with Zr(Ⅳ)on MGLW to develop a stable chemical bond by ion exchange,resulting in the removal of fluoride.
引文
[1]Mohapatra M,Anand S,Mishra B K,et al.Review of fluoride removal from drinking water[J].Journal of Environmental Management,2009(91):67-77.
[2]Chinoy N J.Effects of fluoride on physiology of animals and human beings[J].Indian J Environ Toxicol,1991,25(1):17-32.
[3]陈后兴,罗仙平,刘立良.含氟废水处理研究进展[J].四川有色金属,2006(1):31-35.
[4]Lai Y D,Liu J C.Fluoride removal from water with spent catalyst[J].Separation Science and Technology,1996,31(20):2791-2803.
[5]周珏明,余春香.吸附法处理含氟废水的研究进展[J].离子交换与吸附,2001,17(5):369-376.
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[7]Huang C Jane,Liu J C.Precipitate-flotation of fluoride-containing wastewater from a semiconductor manufacturer[J].Wat Res,1999,33(16):3403-3412.
[8]Liu Ruiping,Zhu Lijun,Gong Wenxin.Effects of fluoride on coagulation performance of aluminum chloride towards Kaolin suspension[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2013(421):84-90.
[9]Liu Ruixia,Guo Jinlong,Tang Hongxiao.Adsorption of fluoride,phosphate and arsenate ions on a new type of ion exchange fiber[J].Journal of Colloid and Interface Science,2002(248):268-274.
[10]Imen Bejaoui,Amine Mnif,Béchir Hamrouni.Performance of reverse osmosis and nanofiltration in the removal of fluoride from model water and metal packaging industrial effluent[J].Separation Science and Technology,2014(49):1135-1145.
[11]Zakia Amof,Bernard Barioub,Nabil Mameri,et al.Fluoride removal from brackish water by electrodialysis[J].Desalination,2001(133):215-223.
[12]Shihabudheen M Maliyekkal,Sanjay Shukla,Ligy Philip,et al.Enhanced fluoride removal from drinking water by magnesia-amended activated alumina granules[J].Chemical Engineering Journal,2008(140):183-192.
[13]廖学品.基于皮胶原纤维的吸附材料制备及吸附特性研究[D].成都:四川大学,2006:1-5.
[14]丁云,廖学品,石碧.胶原纤维固载锆(Ⅳ)对含氟、磷废水中磷的去除[J].皮革科学与工程,2007,17(1):6-10.Ding Yun,Liao Xuepin,Shi Bi.Removal of phosphorus from PO43-and F-containing wastewater by Zr(Ⅳ)immobilized on collagen fiber[J].Leather Science and Engineering,2007,17(1):6-10.(in Chinese)
[15]Piccin J S,Gomes C S,Feris L A,et al.Kinetics and isotherms of leather dye adsorption by tannery solid waste[J].Chemical Engineering Journal,2012(183):30-38.
[16]Qiang Taotao,Luo Min,Bu Qiaoqiao.Adsorption of an acid dye on hyperbranched aminated collagen fibers[J].Chemical Engineering Journal,2012(197):343-349.
[17]Xu Qunjie,Ju Yanzhong,Ge Honghua.Study on adsorption property of collagen fiber loaded hyperbranched polyamideamine toward Cr(Ⅵ)[J].Advanced Materials Research,2012(610/611/612/613):514-517.
[18]王学川,张斐斐,强涛涛.超支化胶原纤维吸附剂对Cr(VI)的吸附特性和机理研究[J].化学学报,2012(70):2536-2542.Wang Xuechuan,Zhang Feifei,Qiang Taotao.Characteristic and adsorption mechanism of hyperbranched collagen fiber toward Cr(Ⅵ)[J].Acta Chimica Sinica,2012(70):2536-2542.(in Chinese)
[19]Qiang Taotao,Bu Qiaoqiao,Ren Longfang,et al.Adsorption behaviors of Cr(Ⅲ)on carboxylated collagen fiber[J].Journal of Applied Polymer Science,2014:40285.
[20]邓慧,廖学品,石碧.胶原纤维负载金属离子对氟的吸附性能研究[J].四川大学学报:工程科学版,2006,38(3):76-80.
[21]邓慧,廖学品.胶原纤维负载锆(Ⅳ)吸附剂的制备及其吸附水中氟离子的研究[J].工业用水与废水,2011,42(6):67-70.Deng Hui,Liao Xuepin.A study of Zr(Ⅳ)immobilized collagen fiber adsorbent preparation and its adsorption performance for fluorine ions in water[J].Industrial Water and Wastewater,2011,42(6):67-70.(in Chinese)
[22]Liao Xuepin,Sh i Bi.Adsorption of fluoride on zirconium(Ⅳ)-impregnated collagen fiber[J].Environment Science and Technology,2005(39):4628-4632.
[23]任涛,廖学品,石碧,等.含铬废革屑负载锆对水中氟的吸附[J].皮革科学与工程,2009,19(3):5-14.Ren Tao,Liao Xuepin,Shi Bi,et al.Adsorption of fluoride from aqueous solution by Zr(Ⅳ)loaded chromic leather waste[J].Leather Science and Engineering,2009,19(3):5-14.(in Chinese)
[24]Wang Jing,Lin Xiaoyan,Luo Xuegang.A sorbent of carboxymethyl cellulose loaded with zirconium for the removal of fluoride from aqueous solution[J].Chemical Engineering Journal,2014(252):415-422.
[25]Han Runping,Zou Weihua,Zhang Zongpei,et al.Removal of copper(Ⅱ)and lead(Ⅱ)from aqueous solution by manganese oxide coated sand I.characterization and kinetic study[J].Journal of Hazardous Materials,2006(B137):384-395.
[26]Dou Xiaomin,Dinesh Mohan,Charles U Pittman Jr.Remediating fluoride from water using hydrous zirconium oxide[J].Chemical Engineering Journal,2012(198/199):236-245.
[27]Legrouri A,Badreddine M,Barroug A.Influence of p H on the synthesis of the Zn-Al-nitrate layered double hydroxide and the exchange of nitrate by phosphate ions[J].Journal of Materials Science Letters,1999(18):1077-1079.
[28]李恩红,强西怀,丁志文,等.超微皮革粉体表面改性的研究[J].中国皮革,2011,40(11):10-13.Li Enhong,Qiang Xihuai,Ding Zhiwen,et al.Surface modification of leather superfine powder[J].China Leather,2011,40(11):10-13.(in Chinese)
[29]王一凡.Ca-Al-La复合除氟材料的制备及其除氟性能研究[D].武汉:武汉理工大学,2012:35-36.
[30]王学川,张斐斐,强涛涛.超支化胶原纤维吸附剂的合成与表征[J].功能材料,2013,44(4):527-531.Wang Xuechuan,Zhang Feifei,Qiang Taotao.Synthesis and characterization of hyperbranched collagen fiber absorbent[J].Journal of Functional Materials,2013,44(4):527-531.(in Chinese)
[31]Zhou Qiusheng,Lin Xiaoyan,Li Bin,et al.Fluoride adsorption from aqueous solution by aluminum alginate particles prepared via electrostatic spinning device[J].Chemical Engineering Journal,2014(256):306-315.
[2]Chinoy N J.Effects of fluoride on physiology of animals and human beings[J].Indian J Environ Toxicol,1991,25(1):17-32.
[3]陈后兴,罗仙平,刘立良.含氟废水处理研究进展[J].四川有色金属,2006(1):31-35.
[4]Lai Y D,Liu J C.Fluoride removal from water with spent catalyst[J].Separation Science and Technology,1996,31(20):2791-2803.
[5]周珏明,余春香.吸附法处理含氟废水的研究进展[J].离子交换与吸附,2001,17(5):369-376.
[6]Miguel A Sandoval,Rosalba Fuentes,JoséL Nava,et al.Fluoride removal from drinking water by electrocoagulation in a continuous filter press reactor coupled to a flocculator and clarifier[J].Separation and Purification Technology,2014(134):163-170.
[7]Huang C Jane,Liu J C.Precipitate-flotation of fluoride-containing wastewater from a semiconductor manufacturer[J].Wat Res,1999,33(16):3403-3412.
[8]Liu Ruiping,Zhu Lijun,Gong Wenxin.Effects of fluoride on coagulation performance of aluminum chloride towards Kaolin suspension[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2013(421):84-90.
[9]Liu Ruixia,Guo Jinlong,Tang Hongxiao.Adsorption of fluoride,phosphate and arsenate ions on a new type of ion exchange fiber[J].Journal of Colloid and Interface Science,2002(248):268-274.
[10]Imen Bejaoui,Amine Mnif,Béchir Hamrouni.Performance of reverse osmosis and nanofiltration in the removal of fluoride from model water and metal packaging industrial effluent[J].Separation Science and Technology,2014(49):1135-1145.
[11]Zakia Amof,Bernard Barioub,Nabil Mameri,et al.Fluoride removal from brackish water by electrodialysis[J].Desalination,2001(133):215-223.
[12]Shihabudheen M Maliyekkal,Sanjay Shukla,Ligy Philip,et al.Enhanced fluoride removal from drinking water by magnesia-amended activated alumina granules[J].Chemical Engineering Journal,2008(140):183-192.
[13]廖学品.基于皮胶原纤维的吸附材料制备及吸附特性研究[D].成都:四川大学,2006:1-5.
[14]丁云,廖学品,石碧.胶原纤维固载锆(Ⅳ)对含氟、磷废水中磷的去除[J].皮革科学与工程,2007,17(1):6-10.Ding Yun,Liao Xuepin,Shi Bi.Removal of phosphorus from PO43-and F-containing wastewater by Zr(Ⅳ)immobilized on collagen fiber[J].Leather Science and Engineering,2007,17(1):6-10.(in Chinese)
[15]Piccin J S,Gomes C S,Feris L A,et al.Kinetics and isotherms of leather dye adsorption by tannery solid waste[J].Chemical Engineering Journal,2012(183):30-38.
[16]Qiang Taotao,Luo Min,Bu Qiaoqiao.Adsorption of an acid dye on hyperbranched aminated collagen fibers[J].Chemical Engineering Journal,2012(197):343-349.
[17]Xu Qunjie,Ju Yanzhong,Ge Honghua.Study on adsorption property of collagen fiber loaded hyperbranched polyamideamine toward Cr(Ⅵ)[J].Advanced Materials Research,2012(610/611/612/613):514-517.
[18]王学川,张斐斐,强涛涛.超支化胶原纤维吸附剂对Cr(VI)的吸附特性和机理研究[J].化学学报,2012(70):2536-2542.Wang Xuechuan,Zhang Feifei,Qiang Taotao.Characteristic and adsorption mechanism of hyperbranched collagen fiber toward Cr(Ⅵ)[J].Acta Chimica Sinica,2012(70):2536-2542.(in Chinese)
[19]Qiang Taotao,Bu Qiaoqiao,Ren Longfang,et al.Adsorption behaviors of Cr(Ⅲ)on carboxylated collagen fiber[J].Journal of Applied Polymer Science,2014:40285.
[20]邓慧,廖学品,石碧.胶原纤维负载金属离子对氟的吸附性能研究[J].四川大学学报:工程科学版,2006,38(3):76-80.
[21]邓慧,廖学品.胶原纤维负载锆(Ⅳ)吸附剂的制备及其吸附水中氟离子的研究[J].工业用水与废水,2011,42(6):67-70.Deng Hui,Liao Xuepin.A study of Zr(Ⅳ)immobilized collagen fiber adsorbent preparation and its adsorption performance for fluorine ions in water[J].Industrial Water and Wastewater,2011,42(6):67-70.(in Chinese)
[22]Liao Xuepin,Sh i Bi.Adsorption of fluoride on zirconium(Ⅳ)-impregnated collagen fiber[J].Environment Science and Technology,2005(39):4628-4632.
[23]任涛,廖学品,石碧,等.含铬废革屑负载锆对水中氟的吸附[J].皮革科学与工程,2009,19(3):5-14.Ren Tao,Liao Xuepin,Shi Bi,et al.Adsorption of fluoride from aqueous solution by Zr(Ⅳ)loaded chromic leather waste[J].Leather Science and Engineering,2009,19(3):5-14.(in Chinese)
[24]Wang Jing,Lin Xiaoyan,Luo Xuegang.A sorbent of carboxymethyl cellulose loaded with zirconium for the removal of fluoride from aqueous solution[J].Chemical Engineering Journal,2014(252):415-422.
[25]Han Runping,Zou Weihua,Zhang Zongpei,et al.Removal of copper(Ⅱ)and lead(Ⅱ)from aqueous solution by manganese oxide coated sand I.characterization and kinetic study[J].Journal of Hazardous Materials,2006(B137):384-395.
[26]Dou Xiaomin,Dinesh Mohan,Charles U Pittman Jr.Remediating fluoride from water using hydrous zirconium oxide[J].Chemical Engineering Journal,2012(198/199):236-245.
[27]Legrouri A,Badreddine M,Barroug A.Influence of p H on the synthesis of the Zn-Al-nitrate layered double hydroxide and the exchange of nitrate by phosphate ions[J].Journal of Materials Science Letters,1999(18):1077-1079.
[28]李恩红,强西怀,丁志文,等.超微皮革粉体表面改性的研究[J].中国皮革,2011,40(11):10-13.Li Enhong,Qiang Xihuai,Ding Zhiwen,et al.Surface modification of leather superfine powder[J].China Leather,2011,40(11):10-13.(in Chinese)
[29]王一凡.Ca-Al-La复合除氟材料的制备及其除氟性能研究[D].武汉:武汉理工大学,2012:35-36.
[30]王学川,张斐斐,强涛涛.超支化胶原纤维吸附剂的合成与表征[J].功能材料,2013,44(4):527-531.Wang Xuechuan,Zhang Feifei,Qiang Taotao.Synthesis and characterization of hyperbranched collagen fiber absorbent[J].Journal of Functional Materials,2013,44(4):527-531.(in Chinese)
[31]Zhou Qiusheng,Lin Xiaoyan,Li Bin,et al.Fluoride adsorption from aqueous solution by aluminum alginate particles prepared via electrostatic spinning device[J].Chemical Engineering Journal,2014(256):306-315.