负载Zr(Ⅳ)的水解废弃皮革对氟离子的吸附性能

doi:10.11949/j.issn.0438-1157.20151238

摘要/Abstract

摘要：

将锆(Ⅳ)负载在通过氢氧化钠(NaOH)水解的粒状废弃皮革上制备出新型氟离子(F^-)吸附剂。采用扫描电子显微镜(SEM)、X射线能量色散光谱分析(EDX)、X射线光电子能谱分析(XPS)、傅里叶变换红外吸收光谱分析(FTIR)等方法研究了该吸附剂对水溶液中F^-的吸附特性及其吸附机理。结果表明:研究条件下,粒状废弃皮革与Zr(NO₃)₄·5H₂O最优的质量比为1:3;该吸附剂对F^-的最优吸附pH为4;该吸附剂对F^-的吸附等温线符合Langmuir方程,拟合得出对F^-的饱和吸附量为30.56 mg·g^-1;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羟基(-OH)与吸附剂中的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。

关键词: 废弃皮革, 负载, 氟离子, 吸附, 离子交换, 吸附剂

Abstract:

A novel adsorbent was prepared from hydrolyzed granular leather waste (ZHGLW) impregnated with Zr(Ⅳ) for fluorion removal. Fluorion adsorption performance and mechanism were investigated by scan electron microscope, energy dispersive analysis of X-ray, X-ray photoelectron spectroscope, and Fourier transform infrared spectroscopy. The results indicate that the optimal mass ratio of hydrolyzed granular leather waste and Zr(NO₃)₄·5H₂O is 1:3 in this study. The maximum removal of fluorion is obtained at pH 3. The isotherm data fit the Langmuir isotherm model well and the obtained maximum fluorion adsorption capacity of the sorbent is 30.56 mg·g^-¹. The kinetics of fluorion adsorption onto ZHGLW follows the pseudo-second-order model. Fluorion adsorption process is a chemisorption process, which can be described as that -OH is replaced by fluorion in the form of ion exchange and a stable chemical bond forms through fluorion and impregnated Zr(Ⅳ). Thus, ZHGLW could be an efficient adsorbent for fluorion.

Key words: granular leather waste, impregnated, fluorion, adsorption, ion exchange, adsorbent

中图分类号:

TQ028.3

曾雪, 罗学刚, 周建. 负载Zr(Ⅳ)的水解废弃皮革对氟离子的吸附性能[J]. 化工学报, 2016, 67(4): 1368-1377.

ZENG Xue, LUO Xuegang, ZHOU Jian. Adsorption of fluorion onto hydrolyzed leather waste impregnated with zirconium (Ⅳ)[J]. CIESC Journal, 2016, 67(4): 1368-1377.

参考文献 41

[1]	MOHAPATRA M, ANAND S, MISHRA B K. 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. CHEN H X, LUE X P, LIU L L. Research on the progress of waste water of fluorine containing[J]. Sichuan Nonferrous Metal, 2006, (1): 31-35. DOI: 10.3969/j.issn.1006-4079.2006.01.010.
[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. ZHOU J M, YU C X. Development on dealing with F-containing wastewater using adsorption methods[J]. Ion Exchange and Adsorption, 2001, 17(5): 369-376. DOI: 10.3321/j.issn: 1001-5493. 2001.05.014.
[6]	MIGUEL A S, ROSALBA F, JOSE L N. 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 J, LIU J C. Precipitate-flotation of fluoride-containing waste water from a semiconductor manufacturer[J]. Water Research, 1999, 33(16): 3403-3412.
[8]	LIU R P, ZHU L J, GONG W X. 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 R X, GUO J L, TANG H X. 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 B, AMINE M, BECHIR H. 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 A, BERNARD B, NABIL M, et al. Fluoride removal frorn brackish water by electrodialysis[J]. Desalination, 2001, 133: 215-223.
[12]	MALIYEKKAL S M, SHUKL S, PHILIP L. 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. LIAO X P. Preparations of adsorbents based on collagen fibers and investigations of their adsorption characteristics[D]. Chengdu: Sichuan University, 2006.
[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 Y, LIAO X P, SHI B. 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. DOI: 10.3969/j.issn.1004-7964.2007.01.002.
[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 T T, LUO M, BU Q Q. Adsorption of an acid dye on hyperbranched aminated collagen fibers[J]. Chemical Engineering Journal, 2012, 197: 343-349.
[17]	XU Q J, JU Y Z, GE H H. Study on adsorption property of collagen fiber loaded hyperbranched polyamide-amine toward Cr(Ⅳ)[J]. Advanced Materials Research, 2012, 610-613: 514-517.
[18]	王学川, 张斐斐, 强涛涛. 超支化胶原纤维吸附剂对Cr(Ⅳ)的吸附特性和机理研究[J]. 化学学报, 2012, 70: 2536-2542. WANG X C, ZHANG F F, QIANG T T. Characteristic and adsorption mechanism of hyperbranched collagen fiber toward Cr(Ⅳ)[J]. Acta Chimica Sinica, 2012, 70: 2536-2542. DOI: 10.6023/A12080609.
[19]	DOU X M, ZHANG Y S, WANG H J, et al. Performance of granular zirconium-iron oxide in the removal of fluoride from drinking water[J]. Water Research, 2011, 45: 3571-3578.
[20]	WANG J, LIN X Y, LUO X G. A sorbent of carboxymethyl cellulose loaded with zirconium for the removal of fluoride from aqueous solution[J]. Chemical Engineering Journal, 2014, 252: 415-422.
[21]	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. DENG H, LIAO X P, SHI B. Study on the adsorption properties of fluoride from aqueous solution by metal ions-loaded collagen fiber (MICF)[J]. Journal of Sichuan University (Engineering Science Edition), 2006, 38(3): 76-80.DOI: 10.3969/j.issn.1009-3087. 2006.03.015.
[22]	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 H, LIAO X P. 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. DOI: 10.3969/j.issn.1009-2455.2011.06.017.
[23]	LIAO X P, SHI B. Adsorption of fluoride on zirconium(Ⅳ)-impregnated collagen fiber[J]. Environment Science & Technology, 2005, 39: 4628-4632.
[24]	邓慧, 廖学品, 石碧. 胶原纤维负载铈(CeCF)吸附水体中氟的研究[J]. 皮革科学与工程, 2006, 16(6): 9-14. DENG H, LIAO X P, SHI B. Adsorption of fluoride from aqueous solution by cerium(Ⅲ)-loaded collagen fiber[J]. Leather Science and Engineering, 2006, 16(6): 9-14. DOI: 10.3969/j.issn. 1004-7964. 2006.06.002.
[25]	HAN R P, ZOU W H, ZHANG Z P, 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]	SWAIN S K, PATNAIK T, PATNAIK P C, et al. Development of new alginate entrapped Fe(Ⅲ)-Zr(Ⅳ) binary mixed oxide for removal of fluoride from water bodies[J]. Chemical Engineering Journal, 2013, 215/216: 763-771.
[27]	YADAV A K, ABBASSI R, GUPTA A, et al.Removal of fluoride from aqueous solution and groundwater by wheat straw, sawdust and activated bagasse carbon of sugarcane[J]. Ecological Engineering, 2013, 52: 211-218.
[28]	BARATHI M, KUMAR A S K, RAJESH N. A novel ultrasonication method in the preparation of zirconium impregnated cellulose for effective fluoride adsorption[J]. Ultrason. Sonochem., 2014, 21: 1090-1099.
[29]	PANDI K, VISWANATHAN N. A novel metal coordination enabled in carboxylated alginic acid for effective fluoride removal[J]. Carbohydrate Polymers, 2015, 118: 242-249.
[30]	AUJANA M G, MASHRA A, ACHARYA B C. Hydrous ferric oxide droped alginate beads for fluoride removal: adsorption kinetics and equilibrium studies[J]. Applied Surface Science, 2013, 270: 767-776.
[31]	GANVIR V, DAS K. Removal of fluoride from drinking water using aluminum hydroxide coated rice husk ash[J]. Journal of Hazardous Materials, 2011, 185: 1287-1294.
[32]	LIU J, LI W Y, LIU Y G, et al. Titanium(Ⅳ) hydrate based on chitosan template for defluoridation from aqueous solution[J]. Applied Surface Science, 2014, 293: 46-54.
[33]	CAIA H M, CHEN G J, PENG C Y, et al. Removal of fluoride from drinking water using tea waste loaded with Al/Fe oxides: a novel, safe and efficient biosorbent.[J]. Applied Surface Science, 2015, 328: 34-44.
[34]	PAUDYAL H, PANGENI B, INOUE K, et al. Adsorptive removal of fluoride from aqueous solution using orange waste loaded with multi-valent metal ions[J]. Journal of Hazardous Materials, 2011, 192: 676-682.
[35]	DOU X M, MOHAN D, PITTMAN C U. Remediating fluoride from water using hydrous zirconium oxide[J]. Chemical Engineering Journal, 2012, 198/199: 236-245.
[36]	ROSCA C, POPA M I, LISA G, et al. Interaction of chitosan with natural or synthetic anionic polyelectroltes (Ⅰ): The chitosan-carboxymethylcellulose complex[J]. Carbohyd. Polym., 2005, 62: 35-41.
[37]	SARKAR D, MOHAPATRA D, RAY S, et al. Synthesis and characterization of sol-gel derived ZrO2 doped Al2O3 nanopowder[J]. Ceramics International, 2007, 33: 1275-1282.
[38]	ZHOU Q S, LIN X Y, LI B. Fluoride adsorption from aqueous solution by aluminum alginate particles prepared via electrostatic spinning device[J]. Chemical Engineering Journal, 2014, 256: 306-315.
[39]	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. WANG Y F. Removal of fluoride from aqueous solution on Ca-Al-La composite adsorbent[D]. Wuhan: Wuhan University of Technology, 2012.
[40]	JERE G V, SANTHAMMA M T. IR and laser Raman studies on peroxo fluorospecies of zirconium[J]. Inorganic Chimica Acta, 1977, 24: 57-61.
[41]	LONG F, GONG J L, ZENG G M, et al. Removal of phosphate from aqueous solution by magnetic Fe-Zr binary oxide[J]. Chemical Engineering Journal, 2011, 171: 448-455.