CPAM插层膨润土复合材料的制备及对磷吸附行为
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摘要
分别采用十六烷基三甲基溴化铵(CTMAB)、阳离子聚丙烯酰胺(CPAM)两步湿法成功制备出CPAM插层钠基膨润土(Bent)复合材料(CTMAB/Bent和CPAM/Bent),利用XRD、FESEM、FTIR、BET以及TG-DTG-DSC对材料进行了表征,并进行模拟含磷废水的吸附研究。结果表明:CPAM已稳定插层在Bent的片层结构中,其层间距显著增大,红外光谱出现明显的羰基吸收峰,比表面积减小而表面疏水性增强。含磷废水处理结果表明,吸附性能大小的顺序为CPAM/Bent> CTMAB/Bent> Bent,随着反应温度升高、含磷废水初始浓度增加以及pH降低,CPAM/Bent对磷的去除率逐渐增大,当含磷废水初始质量浓度为3.5 mg/L、pH≈5、温度为35℃、投加量5 g/L,20 min去除率达75%。CPAM/Bent经过5次吸附和再生后,其吸附磷的能力显著下降。吸附等温线均符合Langmuir和Freundlich方程,吸附过程更好地满足准二级动力学方程。
Composite material was synthesized by modifying Na-bentonite(Bent) with hexadecyltrimethylammonium bromide(CTMAB), cationic polyacrylamide(CPAM) through two-step wet method. The samples were characterized by XRD, FESEM, FTIR, BET and TG-DTG-DSC. Then, the adsorption of simulated phosphorous wastewater was investigated. The results indicated that CPAM was intercalated into the lamellar structure of Na-bentonites steadily, the layer spacing was significantly increased. The infrared spectrum showed that the composite material had obvious carbonyl absorption peaks. Its specific surface area decreased and surface hydrophobicity was enhanced after intercalation. The results of adsorption of phosphorous wastewater revealed that the order of adsorbability was CPAM/Bent >CTMAB/Bent > Bent. With the increase of reaction temperature, the initial concentration of phosphorous wastewater and the decrease of pH value, the removal rate of phosphorus by CPAM/Bent was gradually increased. Under the conditions of initial concentration of phosphorous wastewater 3.5 mg/L, pH≈5,temperature 35 ℃, adding amount of CPAM/Bent 5 g/L, and adsorption time 20 min, the removal rate of phosphorus was 75%. After five times adsorption and regeneration, the adsorption ability of CPAM/Bent to phosphorus decreased significantly. The adsorption isotherms could be described by Langmuir and Freundlich equations. The adsorption process could be better satisfied with the pseudo-second order kinetic equation.
Composite material was synthesized by modifying Na-bentonite(Bent) with hexadecyltrimethylammonium bromide(CTMAB), cationic polyacrylamide(CPAM) through two-step wet method. The samples were characterized by XRD, FESEM, FTIR, BET and TG-DTG-DSC. Then, the adsorption of simulated phosphorous wastewater was investigated. The results indicated that CPAM was intercalated into the lamellar structure of Na-bentonites steadily, the layer spacing was significantly increased. The infrared spectrum showed that the composite material had obvious carbonyl absorption peaks. Its specific surface area decreased and surface hydrophobicity was enhanced after intercalation. The results of adsorption of phosphorous wastewater revealed that the order of adsorbability was CPAM/Bent >CTMAB/Bent > Bent. With the increase of reaction temperature, the initial concentration of phosphorous wastewater and the decrease of pH value, the removal rate of phosphorus by CPAM/Bent was gradually increased. Under the conditions of initial concentration of phosphorous wastewater 3.5 mg/L, pH≈5,temperature 35 ℃, adding amount of CPAM/Bent 5 g/L, and adsorption time 20 min, the removal rate of phosphorus was 75%. After five times adsorption and regeneration, the adsorption ability of CPAM/Bent to phosphorus decreased significantly. The adsorption isotherms could be described by Langmuir and Freundlich equations. The adsorption process could be better satisfied with the pseudo-second order kinetic equation.
引文
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[2]Smil V.Phosphorus in the environment:Natural flows and human interferences[J].Annual Review of Energy and the Environment,2003,25(6):53-88.
[3]Falkowski P,Scholes R J,Boyle E,et al.The global carbon cycle:Atest of our knowledge of earth as a system[J].Science,2000,290(13):291-296.
[4]Suneda S T,Ohno T,Soejima K,et al.Simultaneous nitrogen and phosphorus removal using denitrifying phosphate-accumulating organisms in a sequencing batch reactor[J].Biochemical Engineering Journal,2006,27(3):191-196.
[5]Clark T,Stephenson T,Pearce P A.Phosphorus removal by chemical precipitation in a biological aerated filter[J].Water Research,1997,31(10):2557-2563.
[6]Tian S L,Jiang P R,Ning P,et al.Enhanced adsorption removal of phosphate from water by mixed lanthanum/aluminum pillared montmorillonite[J].Chemical Engineering Journal,2009,151(1/2/3):141-148.
[7]Wang Yu(王宇),Gao Baoyu(高宝玉),Yue Wenwen(岳文文),et al.Adsorption kinetics of phosphate from aqueous solutions onto modified corn residue[J].Environmental Science(环境科学),2008,29(3):703-708.
[8]Keskinkan O,Goksu M Z L,Yuceer A,et al.Heavy metal adsorption characteristics of a submerged aquatic plant(myriophyllum spicatum)[J].Process Biochemistry,2003,39(2):179-183.
[9]Boyd S A,Lee J F,Mortland M M.Attenuating organic contaminant mobility by soil modification[J].Nature,1988,333(6171):345-347.
[10]Komadel P.Chemically modified smectites[J].Clay Miner,2003,38(1):127-138.
[11]Shen Y H.Preparations of organobentonite using nonionic surfactants[J].Chemosphere,2001,44(5):989-995.
[12]Lin S H,Juang R S.Heavy metal removal from water by sorption using surfactant-modified montmorillonite[J].Journal of Hazardous Materials,2002,92(3):315-326.
[13]Malakul P,Srinivasan K R,Wang H Y.Metal adsorption and desorption characteristics of surfactant-modified clay complexes[J].Ind Chem Res,1998,37(11):4296-4301.
[14]Ren Jianmin(任建敏),Fu Bianhong(傅遍红),Wu Siwei(吴四维).Properties of adsorption of methyl orange onto intercalated CTMA-Bentonite[J].Journal of Chongqing University(重庆大学学报),2010,33(5):120-124.
[15]Yu Haiqin(于海琴),Yan Liangguo(闫良国),Xin Xiaodong(辛晓东),et al.Synthesis and characterization of CTMAB and PDMDAACmodified organobentonite[J].Spectroscopy and Spectral Analysis(光谱学与光谱分析),2011,31(5):1393-1396.
[16]Sun Jie(孙杰),Zhao Xinzheng(赵新正),Zeng Pei(曾沛).Adsorption properties of cationic polyacrylamide modified bentonite for indigo blue[J].Research of Environmental Sciences(环境科学研究),2013,26(9):1001-1005.
[17]Ren Haibei(任海贝),Li Mingyu(李明玉).Decoloring performance of compound intercalary organo-bentonite modified with cationic polyacrylamide[J].Technology of Water Treatment(水处理技术),2005,31(12):13-15.
[18]Wang T,Zhu J X,Zhu R L,et al.Enhancing the sorption capacity of CTMA-bentonite by simultaneous intercalation of cationic polyacrylamide[J].Journal of Hazardous Materials,2010,178(1/2/3):1078-1084.
[19]Zhu R L,Wang T,Zhu J X,et al.Structural and sorptive characteristics of the cetyltrimethylammonium and polyacrylamide modified bentonite[J].Chemical Engineering Journal,2010,160(1):220-225.
[20]Moreno M,Benavente E,Gonzalez G,et al.Functionalization of bentonite by intercalation of surfactants[J].Molecular Crystals and Liquid Crystals,2006,448(1):123-131.
[21]Chubar N I,Kanibolotskyy V A,Strelko V V,et al.Adsorption of phosphate ions on novel inorganic ion exchangers[J].Colloids and Surfaces A Physicochemical and Engineering Aspects,2005,255(1):55-63.
[22]Chowdhury S R,Yanful E K.Arsenic and chromium removal by mixed magnetite-maghemite nanoparticles and the effect of phosphate on removal[J].Journal of Environmental Management,2010,91(11):2238-2247.
[23]Khenifi A,Bouberka Z,Sekrane F,et al.Adsorption study of an industrial dye by an organic clay[J].Adsorption-journal of the International Adsorption Society,2007,13(2):149-158.