多壁碳纳米管/纳米四氧化三铁-聚乙烯醇微球的制备及其吸附性能研究
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摘要
为去除水体中不同类型污染物,制备了一种多功能的多壁碳纳米管(MWCNTs)/纳米四氧化三铁(Fe_3O_4)-聚乙烯醇(PVA)微球(MWCNTs/Fe_3O_4-PVA)微球,并对MWCNTs/Fe_3O_4-PVA微球进行了表征,探索MWCNTs/Fe_3O_4-PVA微球对铜离子(Cu~(2+))和磺胺嘧啶(SM)的吸附性能。研究结果表明:制得的MWCNTs/Fe_3O_4-PVA微球饱和磁通量为16.18eum/g;在初始温度为25℃,MWCNTs/Fe_3O_4-PVA微球用量为1g/L条件下,Cu~(2+)溶液初始pH=10,吸附平衡时间为4h,MWCNTs/Fe_3O_4-PVA微球对Cu~(2+)的吸附率最高达到96.5%,平衡吸附量达到76mg/g;SM溶液初始pH=4,吸附平衡时间为2h,MWCNTs/Fe_3O_4-PVA微球对SM的吸附率最高达到65.9%,平衡吸附量达到43mg/g。制得的MWCNTs/Fe_3O_4-PVA微球对Cu~(2+)和SM具有较好的吸附性能。
Multi-walled carbon nanotubes(MWCNTs)and Fe_3O_4 nanoparticles-polyvinyl alcohol(Fe_3O_4-PVA)microspheres were composited to adsorb different kinds of water pollutants.MWCNTs/Fe_3O_4-PVA were developed via three steps:1.Fe_3O_4-PVA microspheres prepared by the inverse suspension cross-linked reaction were animated;2.MWCNTs were carboxylated;3.through the esterification reaction,MWCNTs and Fe_3O_4-PVA microspheres were composited.The morphology,composition and magnetism of MWCNTs/Fe_3O_4-PVA were characterized by FT-IR,XPS and VSM.The application of adsorption properties on copper ions and sulfadiazine in water were investigated.The results showed that MWCNTs/Fe_3O_4-PVA with saturation magnetization intensity of 16.18 emu/g were prepared successfully.The adsorption balance time for copper ions and sulfadiazine was 4 hand 2 h(T=25℃,the dosage was1 g/L)respectivelly.For copper ions,the maximal adsorption rate was 96.5%(pH=10)and the adsorption capacity was 76 mg/g(pH=10).While for sulfadiazine,the maximal adsorption rate was 65.9%(pH=4)and the adsorption capacity was 43 mg/g(pH=4).
Multi-walled carbon nanotubes(MWCNTs)and Fe_3O_4 nanoparticles-polyvinyl alcohol(Fe_3O_4-PVA)microspheres were composited to adsorb different kinds of water pollutants.MWCNTs/Fe_3O_4-PVA were developed via three steps:1.Fe_3O_4-PVA microspheres prepared by the inverse suspension cross-linked reaction were animated;2.MWCNTs were carboxylated;3.through the esterification reaction,MWCNTs and Fe_3O_4-PVA microspheres were composited.The morphology,composition and magnetism of MWCNTs/Fe_3O_4-PVA were characterized by FT-IR,XPS and VSM.The application of adsorption properties on copper ions and sulfadiazine in water were investigated.The results showed that MWCNTs/Fe_3O_4-PVA with saturation magnetization intensity of 16.18 emu/g were prepared successfully.The adsorption balance time for copper ions and sulfadiazine was 4 hand 2 h(T=25℃,the dosage was1 g/L)respectivelly.For copper ions,the maximal adsorption rate was 96.5%(pH=10)and the adsorption capacity was 76 mg/g(pH=10).While for sulfadiazine,the maximal adsorption rate was 65.9%(pH=4)and the adsorption capacity was 43 mg/g(pH=4).
引文
[1]Zhu C Q,Liu F Q,Zhang Y H,et al.Nitrogen-doped chitosanFe(Ⅲ)composite as a dual-functional material for synergistically enhanced co-removal of Cu(Ⅱ)and Cr(Ⅵ)based on adsorption and redox[J].Chemical Engineering Journal,2016,306:579-587.
[2]Genc-Fuhrman H,Mikkelsen P S,Ledin A.Simultaneous.removal of As,Cd,Cr,Cu,Ni and Zn from stormwater:experimental comparison of 11different sorbents[J].Water Research,2007,41:591-602.
[3]杨梖,白雪,顾海鑫.磁性吸附材料的制备及其在污水处理中的应用[J].环境工程,2015(4):25-29.
[4]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):3888-3894.
[5]Xie J,Meng W,Wu D,et al.Removal of organic pollutants by surfactant modified zeolite:comparison between ionizable phenolic compounds and non-ionizable organic compounds[J].Journal of Hazardous Materials,2012,231/232:57-63.
[6]疏瑞文,杨莹莹,王鑫,等.PAM/AMPS/GO纳米复合水凝胶的制备及染料吸附性能研究[J].化工新型材料,2016,44(7):161-163.
[7]陈守刚,刘丹,王洪芬.改性碳纳米管/壳聚糖复合材料的制备及防污性能[J].化工学报,2016,66(11):4689-4695.
[8]Chen M,Qin X,Zeng G.Single-walled carbon nanotube release affects the microbial enzyme-catalyzed oxidation processes of organic pollutants and lignin model compounds in nature[J].Chemosphere,2016,163:217-226.
[9]Yu J G,Zhao X H,Yang H,et al.Aqueous adsorption and removal of organic contaminants by carbon nanotubes[J].Science of the Total Environment,2014,482/483:241-251.
[10]王莹,贺岩峰.利用碳纳米管吸附溶液中金属离子的研究进展[J].化工新型材料,2010,38(3):32-33.
[11]Zhou Lixin,Pan Shengdong,Chen Xiaohong,et al.Kinetics and thermodynamics studies of pentachlorophenol adsorption on covalently functionalized Fe3O4@SiO2-MWCNTs coreshell magnetic microspheres[J].Chemical Engineering Journal,2016,257:10-19.
[12]Huang Z,Chen G,Zeng G,et al.Polyvinyl alcohol-immobilized phanerochaete chrysosporium and its application in the bioremediation of composite-polluted wastewater[J].Journal of Hazardous Materials,2015,289:174-183.
[13]Zhao D,Yu Y,Chen J P.Treatment of lead contaminated water by a PVDF membrane that is modified by zirconium,phosphate and PVA[J].Water Research,2016,101:564-573.
[14]Rashidi S,Ataie A.Structural and magnetic characteristics of PVA/CoFe2O4nano-composites prepared via mechanical alloying method[J].Materials Research Bulletin,2016,80:321-328.
[15]Mallakpour S,Javadpour M.An innovative strategy for the production of novel magnetite poly(vinyl alcohol)nanocomposite films with double-capped synthesized Fe3O4nanoparticles with citric acid and vitamin C[J].Composite Interfaces,2015,22(9):867-884.
[16]Bai X,Yang B,Gu H,et al.Design of multi-N-functional magnetic PVA microspheres for the rapid removal of heavy metal ions with different valence[J].Desalination and Water Treatment,2015,56(7):1809-1819.
[17]Hua Z L,Yang B,Chen W,et al.Surface functionalized magnetic PVA microspheres for rapid naked-eye recognizing of copper(Ⅱ)ions in aqueous solutions[J].Applied Surface Science,2014,317:226-235.
[18]Bai X,Ye Z F,Qu Y Z,et al.Immobilization of nanoscale Fe-0in and on PVA microspheres for nitrobenzene reduction[J].Journal of Hazardous Materials,2009,172:1357-1364.
[19]Yang W B,Zheng F F,Xue X X.Investigation into adsorption mechanisms of sulfonamides onto porous adsorbents[J].Journal of Colloid and Interface Science,2011,362(2):503-509.
[2]Genc-Fuhrman H,Mikkelsen P S,Ledin A.Simultaneous.removal of As,Cd,Cr,Cu,Ni and Zn from stormwater:experimental comparison of 11different sorbents[J].Water Research,2007,41:591-602.
[3]杨梖,白雪,顾海鑫.磁性吸附材料的制备及其在污水处理中的应用[J].环境工程,2015(4):25-29.
[4]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):3888-3894.
[5]Xie J,Meng W,Wu D,et al.Removal of organic pollutants by surfactant modified zeolite:comparison between ionizable phenolic compounds and non-ionizable organic compounds[J].Journal of Hazardous Materials,2012,231/232:57-63.
[6]疏瑞文,杨莹莹,王鑫,等.PAM/AMPS/GO纳米复合水凝胶的制备及染料吸附性能研究[J].化工新型材料,2016,44(7):161-163.
[7]陈守刚,刘丹,王洪芬.改性碳纳米管/壳聚糖复合材料的制备及防污性能[J].化工学报,2016,66(11):4689-4695.
[8]Chen M,Qin X,Zeng G.Single-walled carbon nanotube release affects the microbial enzyme-catalyzed oxidation processes of organic pollutants and lignin model compounds in nature[J].Chemosphere,2016,163:217-226.
[9]Yu J G,Zhao X H,Yang H,et al.Aqueous adsorption and removal of organic contaminants by carbon nanotubes[J].Science of the Total Environment,2014,482/483:241-251.
[10]王莹,贺岩峰.利用碳纳米管吸附溶液中金属离子的研究进展[J].化工新型材料,2010,38(3):32-33.
[11]Zhou Lixin,Pan Shengdong,Chen Xiaohong,et al.Kinetics and thermodynamics studies of pentachlorophenol adsorption on covalently functionalized Fe3O4@SiO2-MWCNTs coreshell magnetic microspheres[J].Chemical Engineering Journal,2016,257:10-19.
[12]Huang Z,Chen G,Zeng G,et al.Polyvinyl alcohol-immobilized phanerochaete chrysosporium and its application in the bioremediation of composite-polluted wastewater[J].Journal of Hazardous Materials,2015,289:174-183.
[13]Zhao D,Yu Y,Chen J P.Treatment of lead contaminated water by a PVDF membrane that is modified by zirconium,phosphate and PVA[J].Water Research,2016,101:564-573.
[14]Rashidi S,Ataie A.Structural and magnetic characteristics of PVA/CoFe2O4nano-composites prepared via mechanical alloying method[J].Materials Research Bulletin,2016,80:321-328.
[15]Mallakpour S,Javadpour M.An innovative strategy for the production of novel magnetite poly(vinyl alcohol)nanocomposite films with double-capped synthesized Fe3O4nanoparticles with citric acid and vitamin C[J].Composite Interfaces,2015,22(9):867-884.
[16]Bai X,Yang B,Gu H,et al.Design of multi-N-functional magnetic PVA microspheres for the rapid removal of heavy metal ions with different valence[J].Desalination and Water Treatment,2015,56(7):1809-1819.
[17]Hua Z L,Yang B,Chen W,et al.Surface functionalized magnetic PVA microspheres for rapid naked-eye recognizing of copper(Ⅱ)ions in aqueous solutions[J].Applied Surface Science,2014,317:226-235.
[18]Bai X,Ye Z F,Qu Y Z,et al.Immobilization of nanoscale Fe-0in and on PVA microspheres for nitrobenzene reduction[J].Journal of Hazardous Materials,2009,172:1357-1364.
[19]Yang W B,Zheng F F,Xue X X.Investigation into adsorption mechanisms of sulfonamides onto porous adsorbents[J].Journal of Colloid and Interface Science,2011,362(2):503-509.