Synthesis of magnetic cationic chitosan flocculant by low-pressure UV light for the removal of Cr(Ⅵ)
ZHENG Huai-li1, ZHONG Zheng1, ZOU Hong2, BAI Ying3, ZHAO Rui1, DING Wei1, JIANG Jun-yi1
1. Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, State Ministry of Education, Chongqing University, Chongqing 400045, China; 2. Chongqing Lanjie Guangshun Water Treatment Materials Co. Ltd, Chongqing 402465, China; 3. CenerTech Tianjin Chemical Research and Design Institute Co. Ltd, Tianjin 300131, China
Abstract：A new magnetic chitosan flocculant FSCAD was synthesized by using magnetic Fe3O4 coated with silica and silane coupling agent (KH-570) as magnetic core, chitosan, acrylamide and acryloyloxyethyl trimethylammonium chloride as graft monomers and low-pressure ultraviolet light as initiator, the Cr(Ⅵ) removal properties of the material were studied. The flocculants were characterized by fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray diffractometer and vibration sample magnetometer, showing the materials were successfully prepared and have good magnetic response. The effects of pH, dosage, reaction time and interference ions on flocculation properties were explored and fitted to the flocculation dynamics model. The flocculation kinetics accorded with the pseudo second order kinetic equation and the removal effect of FSCAD on low concentration Cr(Ⅵ) wastewater reached 90.48% at the added amount of 900mg/L, pH of 3 and the reaction time of 60min.
Marikkani S, Kumar J V, Muthuraj V. Design of novel solar-light driven sponge-like Fe2V4O13 photocatalyst:A unique platform for the photoreduction of carcinogenic hexavalent chromium[J]. Solar Energy, 2019,188:849-856.
[2]
Zi H L, Shu Y X, Guang H X, et al. Removal of hexavalent chromium from groundwater using sodium alginate dispersed nano zero-valent iron[J]. Journal of Environmental Management, 2019,244:33-39.
[3]
Chang J J, Wang H, Zhang J,et al. New insight into adsorption and reduction of hexavalent chromium by magnetite:Multi-step reaction mechanism and kinetic model developing[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2021,611:125784.
[4]
Xiao D H, Pei Y L. Surface Water Pollution in the Middle Chinese Loess Plateau with Special Focus on Hexavalent Chromium (Cr6+):Occurrence, Sources and Health Risks[J]. Exposure and Health, 2020:385-401.
[5]
Park S H, Shin S S, Park C H, et al. Poly(acryloyl hydrazide) -grafted cellulose nanocrystal adsorbents with an excellent Cr(VI) adsorption capacity[J]. Journal of Hazardous Materials, 2020,394:122512.
[6]
Jiang Z K, Chen K X, Zhang Y C, et al. Dionysiou. Magnetically recoverable MgFe2O4/conjugated polyvinyl chloride derivative nanocomposite with higher visible-light photocatalytic activity for treating Cr(VI) -polluted water[J]. Separation and Purification Technology, 2020,236:116272.
[7]
Ge T, Jiang Z K, Shen Li, et al. Synthesis and application of Fe3O4/FeWO4 composite as an efficient and magnetically recoverable visible light-driven photocatalyst for the reduction of Cr(VI)[J]. Separation and Purification Technology, 2021,263:118401.
[8]
Ren Y F, Han Y H, Lei X F, et al. A magnetic ion exchange resin with high efficiency of removing Cr (VI)[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2020,604:125279.
[9]
Zhang Y H, Xu X M, Yue C L, et al. Insight into the efficient co-removal of Cr(VI) and Cr(III) by positively charged UiO-66-NH2 decorated ultrafiltration membrane[J]. Chemical Engineering Journal, 2021,404:126546.
[10]
王刚,常青,杜凤龄,等. pH值对新型高分子螯合絮凝剂捕集Cr(Ⅲ)和Cr(Ⅵ)的影响[C]//中国环境科学学会、四川大学.2014中国环境科学学会学术年会论文集(第五章).中国环境科学学会、四川大学:中国环境科学学会, 2014:336-342. Wang G, Chang Q, Du F L, et al. Effect of pH values on novel polymer chelate flocculants that trap Cr(Ⅲ) and Cr(Ⅵ)[C]//Chinese Society For Environmental Sciences, Sichuan University. Proceedings of the 2014 Annual Meeting of Chinese Society For Environmental Sciences (Chapter V). Chinese Society For Environmental Sciences, Sichuan University:Chinese Society of Environmental Sciences, 2014:336-342.
[11]
Zheng H, Ma J, Zhu C, et al. Synthesis of anion polyacrylamide under UV initiation and its application in removing dioctyl phthalate from water through flocculation process[J]. Separation and Purification Technology, 2014,123:35-44.
[12]
Kyzas G Z, Siafaka P I, Lambropoulou D A, et al. Poly(itaconic acid) -grafted chitosan adsorbents with different cross-linking for Pb(II) and Cd(II) uptake[J]. Langmuir, 2014,30(1):120-131.
[13]
刘冰枝.聚羧酸-壳聚糖基新型絮凝剂及应用性能研究[D]. 重庆:重庆大学, 2018. Liu B Z. Preparation of novel polycarboxylate−chitosan based flocculant and application performance[D]. Chongqing:Chongqing University, 2018.
[14]
郑怀礼,蒋君怡,万鑫源,等.磁性纳米颗粒的制备及其复合材料吸附处理工业废水的研究进展[J]. 中国环境科学, 2021,41(5):1-14. Zheng H L, Jiang J Y, Wan X Y, et al. A research progress on preparation of magnetic nanoparticles and adsorption treatment of their composites in industrial wastewater[J]. China Environmental Science, 2021,41(5):1-14.
[15]
吴江渝,许谦,李竹,等.磁性二氧化硅纳米粒子的制备及性能[J]. 武汉工程大学学报, 2014,36(7):43-7. Wu J Y, Xu Q, LI Z, et al. Preparation and properties of magnetic silica nanoparticles[J]. Journal of Wuhan University of Engineering, 2014, 36(7):43-47.
[16]
Borsagli F G L M, Mansur A A P, Chagas P, et al. O-carboxymethyl functionalization of chitosan:Complexation and adsorption of Cd (II) and Cr (VI) as heavy metal pollutant ions[J]. Reactive & Functional Polymers, 2015,97:37-47.
[17]
Copello G J, Varela F, Vivot R M, et al. Immobilized chitosan as biosorbent for the removal of Cd(II), Cr(III) and Cr(VI) from aqueous solutions[J]. Bioresource technology, 2008,99(14):6538-6544.
[18]
付坤.低压光引发阳离子聚丙烯酰胺制备及其絮凝性能研究[D]. 安徽工业大学, 2017. Fu K. Study on preparation and flocculation properties of low pressure lighe induced cationic polyacrylamide[D]. Anhui University of Technology, 2017.
[19]
Alqadami A A, Naushad M, Abdalla M A, et al. Efficient removal of toxic metal ions from wastewater using a recyclable nanocomposite:A study of adsorption parameters and interaction mechanism[J]. Journal of Cleaner Production, 2017,156:426-436.
[20]
GB/T 9723-2007化学试剂火焰原子吸收光谱法通则[S]. GB/T 9723-2007 Chemical flame atomic absorption spectrometry[S].
[21]
Yan Z, Yang H, Ouyang J, et al. In situ loading of highly-dispersed CuO nanoparticles on hydroxyl group-rich SiO2-AlOOH composite nanosheets for CO catalytic oxidation[J]. Chemical Engineering Journal, 2017,316:1035-1046.
[22]
Li K, Wang Y, Huang M, et al. Preparation of chitosan-graft-polyacrylamide magnetic composite microspheres for enhanced selective removal of mercury ions from water[J]. Journal of Colloid and Interface Science, 2015,455:261-270.
[23]
Li X, Zheng H, Wang Y, et al. Fabricating an enhanced sterilization chitosan-based flocculants:Synthesis, characterization, evaluation of sterilization and flocculation[J]. Chemical Engineering Journal, 2017,319:119-130.
[24]
Kong Z Y, Wei J F, Li Y H, et al. Rapid removal of Cr(VI) ions using quaternary ammonium fibers functioned by 2-(dimethylamino) ethyl methacrylate and modified with 1-bromoalkanes[J]. Chemical Engineering Journal, 2014,254:365-373.
[25]
Yuan B, Shang Y, Lu Y, et al. The Flocculating Properties of Chitosan-graft-Polyacrylamide Flocculants (I) -Effect of the Grafting Ratio[J]. Journal of Applied Polymer Science, 2010,117(4):1876-1882.
[26]
Zheng X, Zheng H, Zhao R, et al. Polymer-Functionalized Magnetic Nanoparticles:Synthesis, Characterization, and Methylene Blue Adsorption[J]. Materials, 2018,11(8):1312.
[27]
Ge Y, Li Y, Zu B, et al. AM-DMC-AMPS Multi-Functionalized Magnetic Nanoparticles for Efficient Purification of Complex Multiphase Water System[J]. Nanoscale Research Letters, 2016,11:217.
[28]
Li L, Lu W, Ding D, et al. Adsorption properties of pyrene-functionalized nano-Fe3O4 mesoporous materials for uranium[J]. Journal of Solid State Chemistry, 2019,270:666-673.
[29]
Usman T M, Su X, Zhao M, et al. Preparation of hydroxypropyl-cyclodextrin-graphene/Fe3O4 and its adsorption properties for heavy metals[J]. Surfaces and Interfaces, 2019,16:43-49.
[30]
邵亚辉.新型阳离子聚丙烯酰胺"水包水"乳液的制备及应用[D]. 广州:华南理工大学, 2020. Shao Y H. Preparation and application of novel cationic polyacrylamide "water-in-water" emulsion[D]. guagnzhou:South China University of Technology, 2020.
[31]
Yang Z L, Gao B Y, Li C X, et al. Synthesis and characterization of hydrophobically associating cationic polyacrylamide[J]. Chemical Engineering Journal, 2010,161(1/2):27-33.
[32]
Zhao C, Zheng H, Feng L, et al. Improvement of Sludge Dewaterability by Ultrasound-Initiated Cationic Polyacrylamide with Microblock Structure:The Role of Surface-Active Monomers[J]. Materials, 2017,10(3):282.
[33]
Xing Y, Zhang J, Chen F, et al. Mesoporous polydopamine nanoparticles with co-delivery function for overcoming multidrug resistance via synergistic chemo-photothermal therapy[J]. Nanoscale, 2017,9(25):8781-8790.
[34]
Feng L, Zheng H, Gao B, et al. Fabricating an anionic polyacrylamide (APAM) with an anionic block structure for high turbidity water separation and purification[J]. Rsc Advances, 2017,7(46):28918-28930.
[35]
Zhao N, Zhao C F, Tsang D C W, et al. Microscopic mechanism about the selective adsorption of Cr(VI) from salt solution on O-rich and N-rich biochars[J]. Journal of Hazardous Materials, 2021,404(PA):124162.
[36]
Zheng C F, Zheng H L, Wang Y J, et al. Synthesis of novel modified magnetic chitosan particles and their adsorption performance toward Cr(VI)[J]. Bioresource Technology, 2018,267:1-8.
[37]
Sharma R K, Kumar R. Functionalized cellulose with hydroxyethyl methacrylate and glycidyl methacrylate for metal ions and dye adsorption applications[J]. International Journal of Biological Macromolecules, 2019,134:704-721.
[38]
Bouza-deano R, Ternero-rodriguez M, Fernandez-espinosa A J. Trend study and assessment of surface water quality in the Ebro River (Spain)[J]. Journal of Hydrology, 2008,361(3/4):227-239.
[39]
Yao Y, Mi N, He C, et al. A novel colloid composited with polyacrylate and nano ferrous sulfide and its efficiency and mechanism of removal of Cr(VI) from Water[J]. Journal of Hazardous Materials, 2020,399:123082.
[40]
Hu Z L, Cai L M, Jiang J M, et al. Green synthesis of expanded graphite/layered double hydroxides nanocomposites and their application in adsorption removal of Cr(VI) from aqueous solution[J]. Journal of Cleaner Production, 2019,209:1216-1227.
[41]
Xie Y Q, Lin J, Liang J, et al. Hypercrosslinked mesoporous poly (ionic liquid) s with high density of ion pairs:Efficient adsorbents for Cr(VI) removal via ion-exchange[J]. Chemical Engineering Journal, 2019,378:122107.
[42]
Khan S, Zhang D, Yang M L, et al. Isotherms, kinetics and thermodynamic studies of adsorption of Ni and Cu by modification of Al2O3 nanoparticles with natural organic matter[J]. Taylor & Francis, 2018,26(3):1422490.
[43]
Sun Y J, Chen A W, Pan S Y, et al. Novel chitosan-based flocculants for chromium and nickle removal in wastewater via integrated chelation and flocculation[J]. Journal of Environmental Management, 2019,248:109241.
[44]
Sun Y J, Chen A W, Sun W Q, et al. Removal of Cu and Cr ions from aqueous solutions by a chitosan based flocculant[J]. Desalination and Water Treatment, 2019,148:256-269.
[45]
Sun Y J, Shah K J, Sun W Q, et al. Performance evaluation of chitosan-based flocculants with good pH resistance and high heavy metals removal capacity[J]. Separation and Purification Technology, 2019,215:286-216.
