河沙载镧复合材料去除水体中磷的研究
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摘要
文章以廉价易得的河沙为载体,采用浸渍法制备得到载镧河沙复合材料,通过批量静态实验研究了载镧河沙对水体中磷酸盐的去除能力,并采用SEM、XRD、XPS进行了表征分析,探讨了去除机理。结果表明,随着载镧河沙投加量的增加,磷酸盐的去除率也随之增加;温度和水体中的共存阴离子对载镧河沙的除磷效果无明显影响;在酸性及中性条件下载镧河沙除磷效果优于碱性条件。载镧河沙对水中磷酸盐的去除过程符合Freundlich等温吸附模型和准二级动力学模型,属于非均相、化学吸附过程。XRD和XPS分析表明,镧以LaOOH的形态成功负载到河沙上,水体中磷酸根主要通过与其表面的羟基基团进行配位体交换作用而实现去除,主要产物为La_4H_3(PO_4)_5。在实际污水处理中,载镧河沙对磷酸盐表现出了高效的选择吸附性能,是一种很有应用前景的除磷剂。
Using sand as the carrier, the lanthanum-coated-sand composites were prepared by impregnation method to remove phosphate from aqueous solution. The samples were analyzed by SEM, XRD, XPS and other analytical methods to reveal the removal mechanism. The result showed that the phosphate removal efficiency increased with the increase in the dosage of lanthanum-coated-sand composites. Temperature and co-existing anions exhibited no significant effects on phosphate removal by the lanthanum-coated-sand composites. The phosphate removal efficiency in acidic and neutral conditions was better than that in alkaline conditions. The removal process of phosphate was in accordance with Freundlich isotherm model and quasi-second order kinetic model, which belongs to a heterogeneous surface and a chemical adsorption process. XRD and XPS analysis showed that lanthanum was successfully loaded into the river sand in the form of LaOOH and phosphate was mainly removed by the ligand exchange between the hydroxyl groups on the surface of the lanthanum-coated-sand composites, and the main product was La_4H_3(PO_4)_5. In the actual sewage treatment, the lanthanum-coated-sand composites for phosphate removal showed a high efficiency of selective adsorption performance, and it was a very promising adsorbent for phosphorus removal in practical application.
Using sand as the carrier, the lanthanum-coated-sand composites were prepared by impregnation method to remove phosphate from aqueous solution. The samples were analyzed by SEM, XRD, XPS and other analytical methods to reveal the removal mechanism. The result showed that the phosphate removal efficiency increased with the increase in the dosage of lanthanum-coated-sand composites. Temperature and co-existing anions exhibited no significant effects on phosphate removal by the lanthanum-coated-sand composites. The phosphate removal efficiency in acidic and neutral conditions was better than that in alkaline conditions. The removal process of phosphate was in accordance with Freundlich isotherm model and quasi-second order kinetic model, which belongs to a heterogeneous surface and a chemical adsorption process. XRD and XPS analysis showed that lanthanum was successfully loaded into the river sand in the form of LaOOH and phosphate was mainly removed by the ligand exchange between the hydroxyl groups on the surface of the lanthanum-coated-sand composites, and the main product was La_4H_3(PO_4)_5. In the actual sewage treatment, the lanthanum-coated-sand composites for phosphate removal showed a high efficiency of selective adsorption performance, and it was a very promising adsorbent for phosphorus removal in practical application.
引文
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[21]Lagergren S.About the theory of so-called adsorption of soluble substances[J].Kungliga Svenska Vetenskapsakademiens,Handlingar,Band,1989,24(4):1-39.
[22]Yeddou M N,Bensmaili A.Kinetics and thermodynamic study of phosphate adsorption on iron hydroxide-eggshell waste[J].Chemical Engineering Journal,2009,147(2/3):87-96.
[23]苗琛琛,毛林强,陶德晶,等.镧改性凹凸棒土的制备及其对水中磷酸盐的吸附[J].环境工程学报,2016,10(12):7069-7074.Miao Chenchen,Mao Linqiang,Tao Dejing,et al.Preparation of lanthanum-modified attapulgite and its adsorption of phosphate from water[J].China Journal of Environmental Engineering,2016,10(12):7069-7074.
[24]Xie J,Wang Z,Lu S Y,et al.Removal and recovery of phosphate from water by lanthanum hydroxide materials[J].Chemical Engineering Journal,2014,254:163-170.
[25]Xie J,Wang Z,Fang D,et al.Green synthesis of a novel hybrid sorbent of zeolite/lanthanum hydroxide and its application in the removal and recovery of phosphate from water[J].Journal of Colloid and Interface Science,2014,423:13-19.
[26]Su Y,Cui H,Li Q,et al.Strong adsorption of phosphate by amorphous zirconium oxide nanoparticles[J].Water Research,2013,47(14):5018-5026.
[27]Lu J B,Liu D F,Hao J,et al.Phosphate removal from aqueous solutions by a nano-structured Fe-Ti bimetal oxide sorbent[J].Chemical Engineering Research and Design,2015,93:652-661.
[2]Tanada S,Kabayama M,Kawasaki N,et al.Removal of phosphate by aluminum oxide hydroxide[J].Journal of Colloid and Interface Science,2003,257(1):135-140.
[3]Lewis L.Scientists Warn of Lack Vital Phosphorous as Biofuels Raise Demand[N].The Times,2008,23.
[4]Ma Z H,Li Q,Yue Q Y,et al.Adsorption removal of ammonium and phosphate from water by fertilizer controlled release agent prepared from wheat straw[J].Chemical Engineering Journal,2011,171(3):1209-1217.
[5]Lu J B,Liu H J,Zhao X,et al.Phosphate removal from water using freshly formed Fe-Mn binary oxide:adsorption behaviors and mechanisms[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2014,455:11-18.
[6]Li G L,Gao S,Zhang G S,et al.Enhanced adsorption of phosphate from aqueous solution by nanostructured iron(Ⅲ)-copper(Ⅱ)binary oxides[J].Chemical Engineering Journal,2014,235:124-131.
[7]陆英,程翔,邢波,等.尿素分解共沉淀法中反应时间对ZnAl类水滑石结构和磷吸附性能的影响[J].环境科学,2012,33(8):2868-2874.Lu Ying,Cheng Xiang,Xing Bo,et al.Influence of reaction time of urea hydrolysis-based co-precipitation on the structure of ZnAl layered double hydroxides and the phosphate adsorption[J].Environmental Science,2012,33(8):2868-2874.
[8]Antelo J,Fiol S,Perez C,et al.Analysis of phosphate adsorption onto ferrihydrite using the CD-MUSIC model[J].Journal of Colloid and Interface Science,2010,347(1):112-119.
[9]Zhang J D,Shen Z M,Shan W P,et al.Adsorption behavior of phosphate on lanthanum(Ⅲ)doped mesoporous silicates material[J].Journal of Environmental Sciences,2010,22(4):507-511.
[10]Zhang L,Zhou Q,Liu J Y,et al.Phosphate adsorption on lanthanum hydroxide-doped activated carbon fiber[J].Chemical Engineering Journal,2012,185/186:160-167.
[11]Guido W,Frank van O,Grant D,et al.Management of eutrophication in Lake De Kuil(The Netherlands)using combined flocculant-lanthanum modified bentonite treatment[J].Water Research,2016,97:83-95.
[12]Joanna G,Magdalena P,Marcin F,et al.Removal of phosphate from water by lanthanum-modified zeolites obtained from fly ash[J].Journal of Colloid and Interface Science,2018,513:72-81.
[13]魏复盛.水和废水监测分析方法[M].北京:中国环境科学出版社,2002:246-248.Wei Fusheng.Water and Wastewater Monitoring Analysis Method[M].Beijing:China Environmental Science Press,2002:246-248.
[14]Ding L,Wu C,Deng H P,et al.Adsorptive characteristics of phosphate from aqueous solutions by MIEX resin[J].Journal of Colloid and Interface Science,2012,376(1):224-232.
[15]Haghseresht F,Wang S,Do D.A novel lanthanum-modified bentonite,Phoslock,for phosphate removal from wastewaters[J].Applied Clay Science,2009,46(4):369-375.
[16]林建伟,王虹,詹艳慧,等.氢氧化镧-天然沸石复合材料对水中低浓度磷酸盐的吸附作用[J].环境科学,2016,37(1):208-219.Lin Jianwei,Wang Hong,Zhan Yanhui,et al.Adsorption of phosphate by lanthanum hydroxide/natural zeolite composites from low concentration phosphate solution[J].Environmental Science,2016,37(1):208-219.
[17]Xie J,Li C,Chi L,et al.Chitosan modified zeolite as a versatile adsorbent for the removal of different pollutants from water[J].Fuel,2013,103(1):480-485.
[18]Zhang G S,Liu H J,Liu R P,et al.Removal of phosphate from water by a Fe-Mn binary oxide adsorbent[J].Journal of Colloid and Interface Science,2009,335(2):168-174.
[19]Ma J,Qi J,Yao C,et al.A novel bentonite-based adsorbent for anionic pollutant removal from water[J].Chemical Engineering Journal,2012,200/201/202(34):97-103.
[20]Wen Z,Zhang Y,Dai C.Removal of phosphate from aqueous solution using nanoscale zerovalent iron(nZVI)[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2014,457(1):433-440.
[21]Lagergren S.About the theory of so-called adsorption of soluble substances[J].Kungliga Svenska Vetenskapsakademiens,Handlingar,Band,1989,24(4):1-39.
[22]Yeddou M N,Bensmaili A.Kinetics and thermodynamic study of phosphate adsorption on iron hydroxide-eggshell waste[J].Chemical Engineering Journal,2009,147(2/3):87-96.
[23]苗琛琛,毛林强,陶德晶,等.镧改性凹凸棒土的制备及其对水中磷酸盐的吸附[J].环境工程学报,2016,10(12):7069-7074.Miao Chenchen,Mao Linqiang,Tao Dejing,et al.Preparation of lanthanum-modified attapulgite and its adsorption of phosphate from water[J].China Journal of Environmental Engineering,2016,10(12):7069-7074.
[24]Xie J,Wang Z,Lu S Y,et al.Removal and recovery of phosphate from water by lanthanum hydroxide materials[J].Chemical Engineering Journal,2014,254:163-170.
[25]Xie J,Wang Z,Fang D,et al.Green synthesis of a novel hybrid sorbent of zeolite/lanthanum hydroxide and its application in the removal and recovery of phosphate from water[J].Journal of Colloid and Interface Science,2014,423:13-19.
[26]Su Y,Cui H,Li Q,et al.Strong adsorption of phosphate by amorphous zirconium oxide nanoparticles[J].Water Research,2013,47(14):5018-5026.
[27]Lu J B,Liu D F,Hao J,et al.Phosphate removal from aqueous solutions by a nano-structured Fe-Ti bimetal oxide sorbent[J].Chemical Engineering Research and Design,2015,93:652-661.