不同类型LDHs负载改性麦饭石对Cr(Ⅵ)吸附性能
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摘要
在碱性条件下采用水热-共沉淀法,将ZnCl_2、MgCl_2和AlCl_3、FeCl_3等不同2价和3价金属化合物两两组合,生成4种层状双金属氢氧化物(LDHs),并负载于天然麦饭石填料表面;分别通过等温吸附试验、解吸附试验、吸附动力学试验、竞争性吸附试验、不同温度及pH值吸附试验,研究LDHs涂层负载改性麦饭石对Cr(Ⅵ)吸附效果的提升作用.结果表明,改性后的各种麦饭石填料对Cr(Ⅵ)的最大理论吸附量均大于天然麦饭石,其中Zn Al-LDHs改性麦饭石对Cr(Ⅵ)的吸附效果最佳,在最适温度15℃时最大理论吸附量接近天然麦饭石的10倍;同时,解吸附试验发现LDHs的负载可以加强填料的重复利用率.所有填料对Cr(Ⅵ)的吸附热力学参数均为ΔGθ<0、ΔHθ<0、ΔSθ> 0,表明填料吸附Cr(Ⅵ)过程为可自发进行的放热过程;LDHs负载改性麦饭石对Cr(Ⅵ)的吸附过程均符合准二级反应过程,以化学吸附为主.通过选用合适的金属离子组合方式制备不同的LDHs负载改性麦饭石,可达到有效提高麦饭石吸附水体中Cr(Ⅵ)性能的目的.
Under alkaline conditions,the hydrothermal coprecipitation method was used to form different layered double hydroxides(LDHs) by combining different bivalent and trivalent metal compounds,such as ZnCl_2,MgCl_2,AlCl_3,and FeCl_3,and then LDHs were coated on the surface of the original maifanite.The effect of LDHs coating-modified maifanite on the improvement of Cr(Ⅵ)adsorption in water was studied using isothermal adsorption,desorption,non-isothermal adsorption,adsorption kinetics,pH,and competitive adsorption tests,respectively.The results show that the maximum theoretical adsorption capacity of modified maifanite for Cr(Ⅵ) is close to ten times that of original maifanite at 15℃.The adsorption effect of Zn Al-LDHs coating-loaded modified maifanite is better than that of other LDHs-coating modified maifanites.In contrast,the results of the desorption experiments show that maifanite coated with LDHs enhances the reuse of substrates.The thermodynamic parameters of the substrate for Cr(Ⅵ) adsorption in the experiment were ΔGθ<0,ΔHθ<0,ΔSθ> 0,indicating that the substrate adsorption process of Cr(Ⅵ) is spontaneous and exothermic.Based on the adsorption kinetics study,the adsorption process of Cr(Ⅵ) by maifanite could be fitted using a pseudosecondary reaction process.The adsorption type was mainly chemisorption.By selecting the suitable metal ion combination method to prepare different LDHs-coating modified maifanites,the Cr(Ⅵ) performance can effectively be improved.
Under alkaline conditions,the hydrothermal coprecipitation method was used to form different layered double hydroxides(LDHs) by combining different bivalent and trivalent metal compounds,such as ZnCl_2,MgCl_2,AlCl_3,and FeCl_3,and then LDHs were coated on the surface of the original maifanite.The effect of LDHs coating-modified maifanite on the improvement of Cr(Ⅵ)adsorption in water was studied using isothermal adsorption,desorption,non-isothermal adsorption,adsorption kinetics,pH,and competitive adsorption tests,respectively.The results show that the maximum theoretical adsorption capacity of modified maifanite for Cr(Ⅵ) is close to ten times that of original maifanite at 15℃.The adsorption effect of Zn Al-LDHs coating-loaded modified maifanite is better than that of other LDHs-coating modified maifanites.In contrast,the results of the desorption experiments show that maifanite coated with LDHs enhances the reuse of substrates.The thermodynamic parameters of the substrate for Cr(Ⅵ) adsorption in the experiment were ΔGθ<0,ΔHθ<0,ΔSθ> 0,indicating that the substrate adsorption process of Cr(Ⅵ) is spontaneous and exothermic.Based on the adsorption kinetics study,the adsorption process of Cr(Ⅵ) by maifanite could be fitted using a pseudosecondary reaction process.The adsorption type was mainly chemisorption.By selecting the suitable metal ion combination method to prepare different LDHs-coating modified maifanites,the Cr(Ⅵ) performance can effectively be improved.
引文
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[2]Owlad M,Aroua M K,Daud W A W,et al.Removal of hexavalent chromium-contaminated water and wastewater:a review[J].Water,Air,and Soil Pollution,2009,200(1-4):59-77.
[3]王刚,杜凤龄,常青,等.新型高分子絮凝剂对废水中Cr(Ⅵ)的捕集性能[J].环境科学,2015,36(5):1707-1712.Wang G,Du F L,Chang Q,et al.Performance of novel macromolecule flocculant in the treatment of wastewater containing Cr(Ⅵ)ions[J].Environmental Science,2015,36(5):1707-1712.
[4]陈友媛,惠红霞,卢爽,等.浒苔生物炭的特征及其对Cr(Ⅵ)的吸附特点和吸附机制[J].环境科学,2017,38(9):3953-3961.Chen Y Y,Hui H X,Lu S,et al.Characteristics of Enteromorpha prolifera biochars and their adsorption performance and mechanisms for Cr(Ⅵ)[J].Environmental Science,2017,38(9):3953-3961.
[5]牛佳.麦饭石的研究现状及发展展望[J].中山大学研究生学刊(自然科学、医学版),2013,34(2):71-77.Niu J.Research situation and development prospect of healing stone[J].Journal of the Graduates Sun Yat-Sen University(Natural Sciences、Medicine),2013,34(2):71-77.
[6]文科,刘国庆,殷艳珍,等.齐齐哈尔碾子山麦饭石岩石矿物学特征研究[J].矿物岩石,2016,36(1):1-7.Wen K,Liu G Q,Yin Y Z,et al.Process mineralogical study on the Maifan stone in Qiqihaer Nianzishan[J].Journal of Mineralogy and Petrology,2016,36(1):1-7.
[7]李娟,张盼月,高英,等.麦饭石的理化性能及其在水质优化中的应用[J].环境科学与技术,2008,31(10):63-66,75.Li J,Zhang P Y,Gao Y,et al.Overview of Maifanshi:its physi-chemical properties and nutritious function in drinking water[J].Environmental Science&Technology,2008,31(10):63-66,75.
[8]陈红,阳旭,赵丽芹,等.不同矿石对反渗透淡化水的调质效果研究[J].浙江大学学报(理学版),2016,43(2):231-236,252.Chen H,Yang X,Zhao L Q,et al.Effect of different ores on water quality adjustment of seawater desalinated by reverse osmosis[J].Journal of Zhejiang University(Science Edition),2016,43(2):231-236,252.
[9]张颖新,周涛,毛娟,等.热改性层状双氢氧化物吸附除Cr(Ⅵ)性能[J].化工学报,2015,66(S1):228-236.Zhang Y X,Zhou T,Mao J,et al.Efficient removal of Cr(Ⅵ)by thermal-modified layered double hydroxides(LDHs):adsorption behaviors,effect parameters and comparison with original LDHs[J].CIESC Journal,2015,66(S1):228-236.
[10]向洋,张翔凌,雷雨,等.不同合成条件对ZnAl-LDHs覆膜改性生物陶粒除磷效果的影响[J].环境科学,2018,39(5):2184-2194.Xiang Y,Zhang X L,Lei Y,et al.Influencing factors for phosphorus removal by modified bio-ceramic substrates coated with Zn Al-LDHs synthesized by different modification conditions[J].Environmental Science,2018,39(5):2184-2194.
[11]张翔凌,黄华玲,郭露,等.Zn系LDHs覆膜改性人工湿地沸石基质除磷机制[J].环境科学,2016,37(8):3058-3066.Zhang X L,Huang H L,Guo L,et al.Mechanisms of phosphorus removal by modified zeolites substrates coated with Zn-LDHs in laboratory-scale vertical-flow constructed wetlands[J].Environmental Science,2016,37(8):3058-3066.
[12]张翔凌,陈俊杰,郭露,等.垂直流人工湿地LDHs覆膜改性沸石基质强化除磷效果及其机制[J].环境科学,2014,35(12):4553-4559.Zhang X L,Chen J J,Guo L,et al.Analysis on the removal efficiency and mechanisms of phosphorus by modified zeolites substrates coated with LDHs reacted by different metal compounds in laboratory-scale vertical-flow constructed wetlands[J].Environmental Science,2014,35(12):4553-4559.
[13]郭露,张翔凌,陈巧珍,等.人工湿地常用生物陶粒基质LDHs覆膜改性及其除磷效果研究[J].环境科学学报,2015,35(9):2840-2849.Guo L,Zhang X L,Chen Q Z,et al.Removal of phosphorus by the modified biological ceramsite coated with different layered double hydroxides in constructed wetlands[J].Acta Scientiae Circumstantiae,2015,35(9):2840-2849.
[14]Zhang X L,Guo L,Huang H L,et al.Removal of phosphorus by the core-shell bio-ceramic/Zn-layered double hydroxides(LDHs)composites for municipal wastewater treatment in constructed rapid infiltration system[J].Water Research,2016,96:280-291.
[15]Zhang X L,Chen Q Z,Guo L,et al.Effects of varying particle sizes and different types of LDH-modified anthracite in simulated test columns for phosphorous removal[J].International Journal of Environmental Research and Public Health,2015,12(6):6788-6800.
[16]Ou J Y,Li H,Yan Z G,et al.In situ immobilisation of toxic metals in soil using Maifan stone and illite/smectite clay[J].Scientific Reports,2018,8(1):4618.
[17]Theiss F L,Ayoko G A,Frost R L.Synthesis of layered double hydroxides containing Mg2+,Zn2+,Ca2+and Al3+layer cations by co-precipitation methods-A review[J].Applied Surface Science,2016,383:200-213.
[18]国家环境保护总局.水和废水监测分析方法[M].(第四版).北京:中国环境科学出版社,2002.
[19]Wang W W,Zhou J B,Achari G,et al.Cr(Ⅵ)removal from aqueous solutions by hydrothermal synthetic layered double hydroxides:adsorption performance,coexisting anions and regeneration studies[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2014,457:33-40.
[20]陈婷.改性麦饭石对水中Cd(Ⅱ)、Cr(Ⅵ)的吸附性能研究[D].成都:成都理工大学,2017.Chen T.Study on adsorption of Cd(Ⅱ)and Cr(Ⅵ)in water by modified medical stone[D].Chengdu:Chengdu University of Technology,2017.
[21]蒋婷婷,喻恺,罗启仕,等.HDTMA改性蒙脱土对土壤Cr(Ⅵ)的吸附稳定化研究[J].环境科学,2016,37(3):1039-1047.Jiang T T,Yu K,Luo Q S,et al.Adsorptive stabilization of soil Cr(Ⅵ)using HDTMA modified montmorillonite[J].Environmental Science,2016,37(3):1039-1047.
[22]Wu X L,Tan X L,Yang S T,et al.Coexistence of adsorption and coagulation processes of both arsenate and NOM from contaminated groundwater by nanocrystallined Mg/Al layered double hydroxides[J].Water Research,2013,47(12):4159-4168.
[23]钟琼,李欢.Mg/Al水滑石微波共沉淀法合成及其对BrO-3吸附性能的研究[J].环境科学,2014,35(4):1566-1575.Zhong Q,Li H.Mg/Al layered double hydroxides prepared by microwave-assisted co-precipitation method for the removal of bromate[J].Environmental Science,2014,35(4):1566-1575.
[24]Sheng G D,Hu J,Li H,et al.Enhanced sequestration of Cr(Ⅵ)by nanoscale zero-valent iron supported on layered double hydroxide by batch and XAFS study[J].Chemosphere,2016,148:227-232.
[25]马叶,刘斌,孙楠,等.改性活性炭对水中铬离子(Ⅵ)的吸附性能[J].环境工程学报,2014,8(7):2672-2676.Ma Y,Liu B,Sun N,et al.Adsorption of Cr ions(Ⅵ)by modified activated carbon[J].Chinese Journal of Environmental Engineering,2014,8(7):2672-2676.
[26]Ma S L,Fan C H,Du L,et al.Intercalation of macrocyclic crown ether into well-crystallized LDH:formation of staging structure and secondary host?guest reaction[J].Chemistry of Materials,2009,21(15):3602-3610.
[27]倪哲明,潘国祥,王力耕,等.LDHs主体层板与卤素阴离子超分子作用的理论研究[J].物理化学学报,2006,22(11):1321-1324.Ni Z M,Pan G X,Wang L G,et al.Theoretical studies on super-molecule interaction between host layer and halide anion of layered double hydroxides[J].Acta Physico-Chimica Sinica,2006,22(11):1321-1324.
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