混凝-超滤预沉积对去除腐殖酸的影响
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摘要
探索利用在膜表面经过混凝预处理,调节膜-颗粒物作用行为的机制,从而改进超滤膜的净水效果是本文的研究核心.研究通过将AlCl_3及Al_(13)两种混凝剂形成的絮体以自然沉降的方式预先沉积在超滤膜表面,考察了对腐殖酸(HA)的去除情况及膜的净水行为.结果表明,使用Al_(13)混凝剂在膜表面沉积的絮体能更好的去除HA,并在一定程度上缓解膜污染,而使用AlCl_3则会加强膜污染现象.随着Al_(13)混凝剂投加量从0.08 mmol·L~(-1)增加到0.18 mmol·L~(-1)时,对HA的去除率也从26%升高到34%,并在超滤膜表面形成预沉积层.在较高投加量0.18 mmol·L~(-1)时,Al_(13)混凝剂在膜表面形成的絮体分形维数(2.45)较AlCl_3(2.29)大,但Al_(13)形成的絮体粒径(300 nm)小于AlCl_3形成的絮体粒径(600 nm),致使在膜表面形成的沉积层相对致密.Zeta电位分析结果表明,Al_(13)混凝剂较AlCl_3混凝剂具有更高的正电荷,较易吸附负电性的HA分子,因此去除HA效果更好,提高膜通量程度更大.
It is important to investigate effects of pre-deposition on removal of humic acid(HA) in the coagulation-ultrafiltration process. The flocs formed by AlCl_3 and Al_(13) were pre-deposited on the surface of ultrafiltration membrane by natural sedimentation, and the removal of HA and the water purification process were investigated. The results showed that the flocs deposited on the surface of the membrane using Al_(13) coagulant could remove HA more efficiently and the membrane fouling could be alleviated, while the use of AlCl_3 would enhance membrane fouling. As the Al_(13) coagulant dosage was increased from 0.08 mmol·L~(-1) to 0.18 mmol·L~(-1), the removal rate of HA was also increased from 26% to 34%. At a higher dosage of 0.18 mmol·L~(-1), the fractal dimension(2.45) of flocs formed by Al_(13) coagulant was larger than that of AlCl_3(2.29), but the floc size(300 nm) formed by Al_(13) was smaller than that of AlCl_3(600 nm). Results of zeta potential showed that Al_(13) had larger amount of positive charges than AlCl_3, and the flocs would adsorb HA molecules more easily.
It is important to investigate effects of pre-deposition on removal of humic acid(HA) in the coagulation-ultrafiltration process. The flocs formed by AlCl_3 and Al_(13) were pre-deposited on the surface of ultrafiltration membrane by natural sedimentation, and the removal of HA and the water purification process were investigated. The results showed that the flocs deposited on the surface of the membrane using Al_(13) coagulant could remove HA more efficiently and the membrane fouling could be alleviated, while the use of AlCl_3 would enhance membrane fouling. As the Al_(13) coagulant dosage was increased from 0.08 mmol·L~(-1) to 0.18 mmol·L~(-1), the removal rate of HA was also increased from 26% to 34%. At a higher dosage of 0.18 mmol·L~(-1), the fractal dimension(2.45) of flocs formed by Al_(13) coagulant was larger than that of AlCl_3(2.29), but the floc size(300 nm) formed by Al_(13) was smaller than that of AlCl_3(600 nm). Results of zeta potential showed that Al_(13) had larger amount of positive charges than AlCl_3, and the flocs would adsorb HA molecules more easily.
引文
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[17] ZEMAITAITIENE R J,ZLIOBAITE E,KLIMAVICIUTE R,et al.The role of anionic substances in removal of textile dyes from solutions using cationic flocculant[J].Colloid Surface A,2003,214 (1-3):37-47.
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[23] LIU T,CHEN Z L,YU W Z,et al,Effect of two-stage coagulant addition on coagulation ultrafiltration process for treatment of humic-rich water [J].Water Research,2011,45(14):4260-4268.
[24] JAVIS P,JEFFERSON B,PARSON S A.Breakage,re-growth and fractal nature of natural organic matter flocs[J].Environmental Science & Technology,2005,39(7),2307-2314.
[2] 陈翔,侯晓庆,郭奏恺,等.超滤膜系统在高碑店再生水厂升级改造中的应用[J].中国给水排水,2018,34(10):77-81.CHEN X,HOU X.Q,GUO Z.K,et al.Application of ultrafiltration membrane system in upgrading and upgrading of gaobeidian reclaimed water plant [J].China Water Supply and Drainage,2018,34 (10):77-81(in Chinese).
[3] 任刚,余燕,杜耀民,等.混凝-超滤处理径流雨水效果——以华南地区为例[J].环境化学,2015,34(6):1142-1149.REN G,YU Y,DU Y M,et al.Coagulation-ultrafiltration treatment of runoff rainwater effect:Taking South China as an example [J].Environmental Chemistry,2015,34(6):1142-1149(in Chinese).
[4] 李政剑,石宝友,王东升.不同粒径粉末活性炭对水中天然有机物吸附性能的比较研究[J].环境科学,2013,34(11):4319-4324.LI Z J,SHI B Y,WANG D S.Comparative study on adsorption properties of natural organic compounds in water by different sizes of powdered activated carbon[J].Environmental Science,2013,34(11):4319-4324(in Chinese).
[5] LI L,GAO N,DENG Y,et al.Characterization of intracellular & extracellular algae organic matters (AOM) of Microcystic aeruginosa and formation of AOM-associated disinfection byproducts and odor & taste compounds[J].Water Research,2012,46(4):1233-1240.
[6] 孙丽华,俞天敏,田海龙,等.典型有机物与超滤膜界面作用及膜污染机制研究[J].环境科学学报,2016,36(2):530-536.SUN L H,YU T M,TIAN H L,et al.Study on the interfacial interaction between typical organic matter and ultrafiltration membrane and membrane fouling mechanism[J].Journal of Environmental Science,2016,36(2):530-536(in Chinese).
[7] 鄢忠森,翟芳术,梁恒,等.超滤膜污染以及膜前预处理技术研究进展[J].膜科学与技术,2014,34(4):108-114.YAN Z S,ZAHI F S,LIANG H,et al.Research progress on ultrafiltration membrane fouling and pre-membrane pretreatment technology [J].Membrane Science and Technology,2014,34(4):108-114(in Chinese).
[8] 刘婷.三种预处理技术对超滤膜污染的影响及其机理研究[D].哈尔滨:哈尔滨工业大学,2011.LIU T.Effect of three pretreatment techniques on ultrafiltration membrane fouling and its mechanism[D].Harbin:Harbin Institute of Technology,2011(in Chinese).
[9] LI K,QU F,LING H,et al.Performance of mesoporous adsorbent resin and powdered activated carbon in mitigating ultrafiltration membrane fouling caused by algal extracellular organic matter[J].Desalination,2014,336:129-137.
[10] 冯萃敏,葛俊男,孙丽华,等.超滤膜表面预沉积吸附剂对膜污染的缓解作用[J].科学技术与工程,2018,18(17):264-271.FENG C M,GE J N,SUN L H,et al.The effect of pre-depositing adsorbent on the surface of ultrafiltration membrane on membrane fouling [J].Science and Technology and Engineering,2018,18(17):264-271(in Chinese).
[11] TEYCHENE B,COLLET G,GLLARD H.Modeling of combined particles and natural organic matter fouling of ultrafiltration membrane [J].Journal of Membrane Science,2016,505:185-193.
[12] SHAO S,FENG Y,YU H,et al.Presence of an adsorbent cake layer improves the performance of gravity-driven membrane (GDM) filtration system [J].Water Research,2017,108:240-249.
[13] WU J,LE-CLECH P,STUETZ R M,et al.Novel filtration mode for fouling limitation in membrane bioreactors [J].Water Research,2008,42(14):3677-3684.
[14] MA B,YU W,JEFFERSON W A,et al.Modification of ultrafiltration membrane with nanoscale zerovalent iron layers for humic acid fouling reduction [J].Water Research,2015,71:140-149.
[15] ASSIYCH S,TABATABAI,SCHIPPERS J C,et al.Effect of coagulation on fouling potential and removal of algal organic matte in ultrafiltration pretreatment to seawater reverse osmosis[J].Water Research,2014,59:283-294.
[16] 董秉直,王洪武,冯晶,等.混凝预处理对超滤膜通量的影响[J].环境科学,2008,29(10):2783-2787.DONG B Z,WANG H W,FENG J,et al.Effect of coagulation pretreatment on ultrafiltration membrane flux [J].Environmental Science,2008,29(10):2783-2787(in Chinese).
[17] ZEMAITAITIENE R J,ZLIOBAITE E,KLIMAVICIUTE R,et al.The role of anionic substances in removal of textile dyes from solutions using cationic flocculant[J].Colloid Surface A,2003,214 (1-3):37-47.
[18] SHIH I,VAN Y,YEH L,et al.Production of a biopolymer flocculant from Bacillus licheniformis and its flocculation properties[J].Bioresource Technol,2001,78(3):267-272.
[19] TURNER R.C,SULAIMAN W.Kinetics of reactions of 8-quinolinolate extraction method and acetate with aluminum species in aqueous solutions.I.Polynuclear hydroxyaluminum cations[J].Can J Chem,1971,49:1683-1687.
[20] ALLOUCHE L,HUGUENARD C,TAULELLE F.3QMAS of three aluminum polycations:space group consistency between NMR and XRD[J].J Phys Chem Solids,2001,62(8):1525-1531.
[21] XU H,JIAO R,XIAO F,et al.Relative importance of hydrolyzed Al species (Ala,Alb,Alc) on residual Al and effects of nano-particles (Fe-surface modified TiO2 and Al2O3) on coagulation[J].Colloid Surface A,2014,446:139-150.
[22] WANG D,SUN W,XU Y,et al.Speciation stability of inorganic polymer flocculant-PACl[J].Colloid Surface A,2004,243 (1-3):1-10.
[23] LIU T,CHEN Z L,YU W Z,et al,Effect of two-stage coagulant addition on coagulation ultrafiltration process for treatment of humic-rich water [J].Water Research,2011,45(14):4260-4268.
[24] JAVIS P,JEFFERSON B,PARSON S A.Breakage,re-growth and fractal nature of natural organic matter flocs[J].Environmental Science & Technology,2005,39(7),2307-2314.
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