基于氮磷废水处理的沸石多孔吸附材料制备
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摘要
以改性沸石粉体为原料,采用添加黏结剂和造孔剂方法制备多孔颗粒沸石,重点研究了黏结剂种类、用量、造孔剂种类和用量,水添加量等对颗粒沸石散失率及吸附氨氮、磷酸盐性能的影响.结果表明:聚乙烯醇(PVA)黏结效果优于水泥和羧甲基纤维素钠(CMC),造孔剂碳酸氢钠相比较活性炭效果更佳.扫描电镜(SEM)结果发现添加碳酸氢钠后,颗粒沸石孔径增大,孔隙结构得到明显改善.在改性沸石粉体中添加1.2%PVA、4%碳酸氢钠、40%水制备所得颗粒型沸石散失率为0,且具有较高氮磷吸附性能,对水中氨氮、磷酸盐的去除率高达88.55%和83.11%.吸附动力学实验表明,多孔颗粒型沸石对氮磷的吸附更加符合拟二级动力学模型.
Porous zeolite particles were prepared by adding adhensive and pore former with modified zeolite powder as raw material.The type and addition of adhensive,type and addition of pore-forming agent,water addition on the loss efficiency of the zeolite particle and the effect of the adsorption of nitrogen and phosphorus were focused on.The results show that polyvinyl alcohol(PVA)was better than cement and sodium carboxymethyl cellulose.The effect of sodiumon bicarbonate was better than that of activated carbon,and the micro-morphology of the porous zeolite particles were observed by scanning electron microscopy(SEM)and the results showed that the pore diameter and pore structure of the zeolite particles were significantly improved after adding sodium bicarbonate.The loss efficiency of porous zeolite particles at 0 was made by adding in the modified zeolite powder 1.2% PVA,4% sodium bicarbonate,40% water.The results showed a high adsorption of nitrogen and phosphorus,and the removal efficiency of nitrogen and that of the phosphorus in wastewater were 88.55% and 83.11%respectively.The adsorption kinetic of nitrogen,phosphorus on porous zeolite particles was following the pseudo-secondorder.
Porous zeolite particles were prepared by adding adhensive and pore former with modified zeolite powder as raw material.The type and addition of adhensive,type and addition of pore-forming agent,water addition on the loss efficiency of the zeolite particle and the effect of the adsorption of nitrogen and phosphorus were focused on.The results show that polyvinyl alcohol(PVA)was better than cement and sodium carboxymethyl cellulose.The effect of sodiumon bicarbonate was better than that of activated carbon,and the micro-morphology of the porous zeolite particles were observed by scanning electron microscopy(SEM)and the results showed that the pore diameter and pore structure of the zeolite particles were significantly improved after adding sodium bicarbonate.The loss efficiency of porous zeolite particles at 0 was made by adding in the modified zeolite powder 1.2% PVA,4% sodium bicarbonate,40% water.The results showed a high adsorption of nitrogen and phosphorus,and the removal efficiency of nitrogen and that of the phosphorus in wastewater were 88.55% and 83.11%respectively.The adsorption kinetic of nitrogen,phosphorus on porous zeolite particles was following the pseudo-secondorder.
引文
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[2]LI R,WANG J J,ZHEN B,et al.Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios[J].Science of the Total Environment,2016,559:121.
[3]LURLING M,WAAJEN G,van OOSTERHOUT F.Humic substances interfere with phosphate removal by lanthanum modified clay in controlling eutrophication[J].Water Research,2014,54:78.
[4]HUANG W,LI D,LIU Z,et al.Kinetics,isotherm,thermodynamic,and adsorption mechanism studies of La(OH)3-modified exfoliated vermiculites as highly efficient phosphate adsorbents[J].Chemical Engineering Journal,2014,236:191.
[5]KOILRAJ P,SASAKI K.Selective removal of phosphate using La-porous carbon composites from aqueous solutions:Batch and column studies[J].Chemical Engineering Journal,2017,317:1059.
[6]DU X,HAN Q,LI J,et al.The behavior of phosphate adsorption and its reactions on the surfaces of Fe-Mn oxide adsorbent[J].Journal of the Taiwan Institute of Chemical Engineers,2017,76:167.
[7]YE Y,HUUH N,GUO W,et al.Insight into biological phosphate recovery from sewage[J].Bioresource Technology,2016,218:874.
[8]YANG S,JIN P,WANG X,et al.Phosphate recovery through adsorption assisted precipitation using novel precipitation material developed from building waste:behavior and mechanism[J].Chemical Engineering Journal,2016,292:246.
[9]MITROGIANNIS D,PSYCHOYOU M,BAZIOTIS I,et al.Removal of phosphate from aqueous solutions by adsorption onto Ca(OH)2 treated natural clinoptilolite[J].Chemical Engineering Journal,2017,320:510.
[10]HUO H,LIN H,DONG Y,et al.Ammonia-nitrogen and phosphates sorption from simulated reclaimed waters by modified clinoptilolite[J].Journal of Hazardous Materials,2012,229:292.
[11]HE Y,LIN H,DONG Y,et al.Preferable adsorption of phosphate using lanthanum-incorporated porous zeolite:Characteristics and mechanism[J].Applied Surface Science,2017,426:995.
[12]WANG S,PENG Y.Natural zeolites as effective adsorbents in water and wastewater treatment[J].Chemical Engineering Journal,2010,156:11.
[13]刘泉利.氧化镧改性硅酸盐矿物的表征及其除磷机理研究[D].北京:北京科技大学,2017.LIU Q L.Study on characterization of lanthanum(III)oxide modifidied silicate minerals and mechanism for phosphorus removal[D].Beijing:University of Science and Technology Beijing,2017.
[14]朱健,王韬远,王平,等.硅藻土基多孔吸附填料的制备及其对Pb2+的吸附[J].中国环境科学,2012,32(12):2205.ZHU Jian,WANG Taoyuan,WANG Ping,et al.Preparation of diatomite-based porous adsorption filler and adsorption on Pb2+[J].China Environmental Science,2012,32(12):2205.
[15]BOWDEN-Green B,BRIENS L.An investigation of drum granulation of biochar powder[J].Powder Technology,2016,288:249.
[16]张秀英.沸石颗粒吸附剂的制备及性能研究[J].金属矿山,2009,401(11):154.ZHANG X Y.Research on the preparation and property of zeolite granular adsorbent[J].Metal Mine,2009,401(11):154.
[17]林海,江乐勇,赵志英,等.市政污水厂二级出水深度脱氮除磷吸附材料[J].北京科技大学学报,2009,31(5):551.LIN H,JIANG L Y,ZHAO Z Y,et al.Adsorption materials of nitrate and phosphate removal in secondary effluent advanced treatment[J].Journal of University of Science and Technology Beijing,2009,31(5):551.
[18]朱海玲,陈沙鸥,李达,等.测定陶瓷材料密度及其气孔率的方法[J].理化检验(物理分册),2006,42(6):289.ZHU Hailing,CHENG Shaou,LI Da,et al.Measuring method for the density and the pore ratio of ceramic materials[J].Physical Testing and Chemical Analysis Part A(Physical Testing),2006,42(6):289.
[19]DHENGE R M,WASHINO K,CARTWRIGHT J J,et al.Twin screw granulation using conveying screws:effects of viscosity of granulation liquids and flow of powders[J].Powder Technology,2013,238:77.
[20]扈玫珑.微细球形TiO2可控制备过程及其动力学研究[D].重庆:重庆大学,2009.HU Meilong.Study on controllable praperation and kinetics of micro spherical titania[D].Chongqing:Chongqing University,2009.
[21]OBRADOVIC N,FILIPOVIC S,MARKOVIC S,et al.Influence of different pore-forming agents on wollastonite microstructures and adsorption capacities[J].Chongqing:Ceramics International,2017,43(10):7461.
[22]ZOU J L,XU G R,LI G B.Ceramsite obtained from water and wastewater sludge and its characteristics affected by Fe2O3,CaO,and MgO[J].Journal of Hazardous Materials,2009,165(1/3):995.
[23]QIN J,CUI C,CUI X,et al.Preparation and characterization of ceramsite from lime mud and coal fly ash[J].Construction&Building Materials,2015,95:10.
[24]KOILRAJ P,SASAKI K.Selective removal of phosphate using La-porous carbon composites from aqueous solutions:batch and column studies[J].Chemical Engineering Journal,2017,317:1059.
[25]CHEN N,FENG C,ZHANG Z,et al.Preparation and characterization of lanthanum(III)loaded granular ceramic for phosphorus adsorption from aqueous solution[J].Journal of the Taiwan Institute of Chemical Engineers,2012,43(5):783.
[26]修瑞瑞,何世颖,宋海亮,等.改性硅藻土负载纳米零价铁去除水中硝酸盐氮[J].化工学报,2016,67(9):3888.XIU R R,HE,S Y,SONG H L et al.Removal of nitrate nitrogen by nanoscale zero-valent iron supported on modified diatomite[J].Journal of Chemical Industry and Engineering,2016,67(9):3888.
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