氨基修饰稻壳生物炭对水溶液中铀的吸附动力学特性
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摘要
为了探究NBC(氨基修饰生物炭)对U(Ⅵ)的吸附性能,通过在BC(未修饰生物炭)上负载氨基的方法得到氨基修饰生物炭,研究BC、NBC对水溶液中U(Ⅵ)的吸附特征,分析生物炭添加量、溶液p H、溶液中阴离子、初始ρ[U(Ⅵ)]、吸附时间和吸附体系温度等因素对U(Ⅵ)吸附的影响,筛选最优的吸附条件,并利用SEM(扫描电镜)、FT-IR(傅里叶红外光谱)、XRD(X-射线衍射)、XPS(X-射线能谱)、BET比表面积、元素分析、零点电位(Zeta电势)测定等手段表征BC、NBC的结构特征,并进一步探讨其对U(Ⅵ)的吸附机理.结果表明:(1)NBC的比表面积和吸附位点显著增加,对U(Ⅵ)的吸附速率和吸附量明显增加,NBC的最大吸附量(69. 63 mg/g)大于BC(53. 95 mg/g).(2)NBC对U(Ⅵ)吸附的最佳条件为生物炭添加量0. 4 g/L、p H 6、初始ρ[U(Ⅵ)]20 mg/L、吸附时间1 h、吸附体系温度328 K.(3)BC、NBC对U(Ⅵ)的吸附动力学均符合伪二级动力学方程,R2均为0. 999;等温吸附过程均符合Sips等温吸附模型,R2均大于0. 914.研究显示,NBC的吸附能力强、环境耐受性好,具有很好的应用潜力.
Amino modified biochars were obtained by loading amino onto rice husk biochar,and adsorption capacities of U( Ⅵ) by these biochars were investigated to reveal the potential use of the modified biochars for U( Ⅵ) adsorption from aqueous solution. The optimal conditions of U( Ⅵ) adsorption such as biochar dosages,p H value of solution,the anion in the solution,initial concentration,adsorption time and temperature were determined. The SEM,FT-IR,XRD,XPS,BET,SA and Zeta potential were used to characterize the properties of biochars and the mechanisms of U( Ⅵ) adsorption. The results showed that:( 1) The specific surface area and adsorption sites of the modified biochar( NBC) were significantly higher than the original biochar( BC),which improves the U( Ⅵ) adsorption capacity of the biochar( Qmax( NBC) = 69. 63 mg/g>Qmax( BC) = 53. 95 mg/g).( 2) The amino modified rice husk biochar had very good removal of U( Ⅵ) when the biochar content was 0. 4 g/L,the initial U( Ⅵ) concentration was 20 mg/L,solution p H was 6,the temperature was 328 K,and the contact time was 1 h.( 3) U( Ⅵ) adsorption kinetics onto the original and modified biochars followed thePseudo Second-Order Kinetic model( R2= 0. 999) and Sipisisotherm model( R2> 0. 914),respectively. The results showed that the modified biochar had high adsorption capacity,good environmental tolerance and better application potential.
Amino modified biochars were obtained by loading amino onto rice husk biochar,and adsorption capacities of U( Ⅵ) by these biochars were investigated to reveal the potential use of the modified biochars for U( Ⅵ) adsorption from aqueous solution. The optimal conditions of U( Ⅵ) adsorption such as biochar dosages,p H value of solution,the anion in the solution,initial concentration,adsorption time and temperature were determined. The SEM,FT-IR,XRD,XPS,BET,SA and Zeta potential were used to characterize the properties of biochars and the mechanisms of U( Ⅵ) adsorption. The results showed that:( 1) The specific surface area and adsorption sites of the modified biochar( NBC) were significantly higher than the original biochar( BC),which improves the U( Ⅵ) adsorption capacity of the biochar( Qmax( NBC) = 69. 63 mg/g>Qmax( BC) = 53. 95 mg/g).( 2) The amino modified rice husk biochar had very good removal of U( Ⅵ) when the biochar content was 0. 4 g/L,the initial U( Ⅵ) concentration was 20 mg/L,solution p H was 6,the temperature was 328 K,and the contact time was 1 h.( 3) U( Ⅵ) adsorption kinetics onto the original and modified biochars followed thePseudo Second-Order Kinetic model( R2= 0. 999) and Sipisisotherm model( R2> 0. 914),respectively. The results showed that the modified biochar had high adsorption capacity,good environmental tolerance and better application potential.
引文
[1]方时姣.低碳经济的实质是能源经济革命[EB/OL].北京:国际能源网,2009-05-20[2009-05-20].http://www.in-en.com.
[2]刘大前,刘恃嵘,王长福,等.活性炭负载纳米零价铁去除水溶液中U(Ⅵ)的研究[J].人工晶体学报,2016,45(5):1328-1334.LIU Daqian,LIU Zhirong,WANG Changfu,et al. Removal of U(Ⅵ)from aqueous solution using nanoscale zero-valent iron supported on activated carbon[J]. Journal of Synthetic Crystals,2016,45(5):1328-1334.
[3] ZHOU Zan,LIU Yunguo,LIU Shaobo,et al. Sorption performance and mechanisms of Arsenic(Ⅴ)removal by magnetic gelatinmodified biochar[J]. Chemical Engineering Journal,2017,314:223-231.
[4] NEWSOME L,MORRIS K,LLOYD J R. The biogeochemistry and bioremediation of uraninm and other priority radionuclides[J].Chemical Geology,2014,363:164-184.
[5] CUI Pang,LIU Yunhai,CAO Xiaohong,et al. Biosorption of Uranium(Ⅵ)from aqueous solution by dead fungal biomass of penicilliumcitrinum[J]. Chemical Engineering Journal,2011,170(1):1-6.
[6]徐佳丽.蒙脱石负载纳米零价铁对水溶液中铀的去除研究[D].武汉:中国地质大学(武汉),2014.
[7]景晨,李义连,徐佳丽,等.高岭土对铀的吸附试验研究[J].安全与环境工程,2014,21(1):73-76.JING Chen,LI Yilian,XU Jiali,et al. Research on the sorption experiment of Uranium on kaolinite[J]. Safety and Environmental Engineering,2014,21(1):73-76.
[8]谢志英,肖化云,王光辉.交联壳聚糖对铀的吸附研究[J].环境工程学报,2010,4(8):1749-1752.XIE Zhiying,XIAO Huayun,WANG Guanghui.Study on adsorption of uranium onto cross-linked chitosan[J]. Chinese Journal of Environmental Engineering,2010,4(8):1749-1752.
[9] LI Zijie,CHEN Fei,YUAN Lilong,et al.Uranium(Ⅵ)adsorption on graphene oxide nanosheets from aqueous solutions[J].Chemical Engineering Journal,2012,210(6):539-546.
[10] HAN Jiangang,FAN Diwu,LI Xiuzhi,et al. Mechanism of Cr6+,Mn2+,Cu2+and Cd2+adsorption by a low-cost rice husk-derived biochar in aqueous solutions[J].Fresenius Environmental Bulletin,2016,25(8):2736-2744.
[11] MA Tianxing,YANG Chen,JIANG Xianying,et al.Adsorption and desorption of Cd(Ⅱ)on amino biochar modified by nano zero valent iron[J]. Chinese Journal of Environmental Engineering,2016,10(10):5433-5439..
[12] WANG Yuying,LU Haohao,LIU Yuxue,et al.Ammonium citratemodified biochar:an adsorbent for La(Ⅲ)ions from aqueous solution[J].Colloids&Surfaces A:Physicochemical&Engineering Aspects,2016,509:550-563.
[13] MA Ying,LIU Wujun,ZHANG Nan,et al. Polyethylenimine modified biochar adsorbent for hexavalent chromium removal from the aqueous solution[J]. Bioresource Technology,2014,169(5):403-408.
[14] WANG Shujuan,GUO Wei,GAO Fan,et al. Characterization and Pb(Ⅱ)removal potential of corn straw-and municipal sludgederived biochars[J]. Royal Society Open Science,2017. doi:10. 1098/rsos. 170402.
[15] YANTASEE W,LIN Yuehe,ALFORRDK L,et al. Electrophilic aromatic substitutions of amine and sulfonate onto fine-grained activated carbon for aqueous-phase metal ion removal[J].Separation Science Technology,2004,39:3263-3279.
[16] HUANG S,CHEN D. Rapid removal of heavy metal cations and anions from aqueoussolutions by an amino-functionalized magnetic nano-adsorbent[J].Journal of Hazardous Materials,2009,163(1):174-179.
[17] LU Huanliang,ZHANG Weihua,YANG Yuxi.Relative distribution of Pb2+sorption mechanisms by sludge-derived biochar[J]. Water Research,2012,46:854-862.
[18] HUANG Xixian,LIU Yunguo,LIU Shaobo,et al.Effective removal of Cr(Ⅵ)usingβ-cyclodextrin-chitosan modified biochars with adsorption/reduction bifuctional roles[J]. Rsc Advances,2015,6(1):94-104.
[19] DING Wenchuan,DONG Xiaoling,MANDU I I. Pyrolytic temperatures impact lead sorption mechanisms by bagasse biochars[J].Chemosphere,2014,105:68-74.
[20] CHUN Yuan,SHENG Guanyao,CHIOUC T,et al.Compositions and sorptive properties of crop residue-derived chars[J].Environmental Science&Technology,2004,38(17):4649-4655.
[21] SCHMIDT M W I,NOAKC A G. Black carbon in soils and sediments:analysis, distribution, implications, and current challenges[J]. Global Biogeochemical Cycles,2000,14(3):777-793.
[22]马亚红,黄婉婷,刁开盛,等.氨化松香基交联聚和树脂对水中诺氟沙星的吸附性能[J].环境科学,2018,39(1):161-169.MA Yahong,HUANG Wanting,DIAO Kaisheng,et al.Evaluation of performance of an aminated rosin-based resin for adsorption of norfloxacin from aqueous solutions[J]. Environmental Science,2018,39(1):161-169.
[23] LAU A Y T,TSHANG D C W,GRAHAM N J D,et al. Surfacemodified biochar in a bioretention system for escherichia coli removal from stormwater[J].Chemosphere,2016,169:89-98.
[24] LIU Shaobo,HUANG Binyan,CHA Liyuan,et al.Enhancement of As(Ⅴ)adsorption from aqueous solution by a magnetic chitosan/biochar composite[J].Rsc Advance,2017,7:10891-10900.
[25] HO Y S,MCKAY G. Pseudo-second order model for sorption processes[J].Process Biochemistry,1999,34(5):451-465.
[26] GONDHALEKAR S C,SHUKLAS R. Equilibrium and kinetics study of Uranium(Ⅵ)from aqueous solution by citrus limetta,peels[J]. Journal of Radioanalytical&Nuclear Chemistry,2014,302(1):451-457.
[27] NASSAR N N. Rapid removal and recovery of Pb(Ⅱ)from wastewater by magnetic nano adsorbents[J]. Journal of Hazardous Materials,2010,184(1/2/3):538-546.
[28] LING Lili,LIU Wujun,ZHANG Shun,et al. Magnesium oxide embedded nitrogen self-doped biochar composites:fast and highefficiency adsorption of heavy metals in an aqueous solution[J].Environmental Science&Technology,2017,51(17):10081-10089.
[29] OYEWO O A,ONYANGO M S,WOLKERSDORFER C.Application of banana peels nanosorbent for the removal of radioactive minerals from real mine water[J]. Journal of Environmental Radioactivity,2016,164:369-376.
[2]刘大前,刘恃嵘,王长福,等.活性炭负载纳米零价铁去除水溶液中U(Ⅵ)的研究[J].人工晶体学报,2016,45(5):1328-1334.LIU Daqian,LIU Zhirong,WANG Changfu,et al. Removal of U(Ⅵ)from aqueous solution using nanoscale zero-valent iron supported on activated carbon[J]. Journal of Synthetic Crystals,2016,45(5):1328-1334.
[3] ZHOU Zan,LIU Yunguo,LIU Shaobo,et al. Sorption performance and mechanisms of Arsenic(Ⅴ)removal by magnetic gelatinmodified biochar[J]. Chemical Engineering Journal,2017,314:223-231.
[4] NEWSOME L,MORRIS K,LLOYD J R. The biogeochemistry and bioremediation of uraninm and other priority radionuclides[J].Chemical Geology,2014,363:164-184.
[5] CUI Pang,LIU Yunhai,CAO Xiaohong,et al. Biosorption of Uranium(Ⅵ)from aqueous solution by dead fungal biomass of penicilliumcitrinum[J]. Chemical Engineering Journal,2011,170(1):1-6.
[6]徐佳丽.蒙脱石负载纳米零价铁对水溶液中铀的去除研究[D].武汉:中国地质大学(武汉),2014.
[7]景晨,李义连,徐佳丽,等.高岭土对铀的吸附试验研究[J].安全与环境工程,2014,21(1):73-76.JING Chen,LI Yilian,XU Jiali,et al. Research on the sorption experiment of Uranium on kaolinite[J]. Safety and Environmental Engineering,2014,21(1):73-76.
[8]谢志英,肖化云,王光辉.交联壳聚糖对铀的吸附研究[J].环境工程学报,2010,4(8):1749-1752.XIE Zhiying,XIAO Huayun,WANG Guanghui.Study on adsorption of uranium onto cross-linked chitosan[J]. Chinese Journal of Environmental Engineering,2010,4(8):1749-1752.
[9] LI Zijie,CHEN Fei,YUAN Lilong,et al.Uranium(Ⅵ)adsorption on graphene oxide nanosheets from aqueous solutions[J].Chemical Engineering Journal,2012,210(6):539-546.
[10] HAN Jiangang,FAN Diwu,LI Xiuzhi,et al. Mechanism of Cr6+,Mn2+,Cu2+and Cd2+adsorption by a low-cost rice husk-derived biochar in aqueous solutions[J].Fresenius Environmental Bulletin,2016,25(8):2736-2744.
[11] MA Tianxing,YANG Chen,JIANG Xianying,et al.Adsorption and desorption of Cd(Ⅱ)on amino biochar modified by nano zero valent iron[J]. Chinese Journal of Environmental Engineering,2016,10(10):5433-5439..
[12] WANG Yuying,LU Haohao,LIU Yuxue,et al.Ammonium citratemodified biochar:an adsorbent for La(Ⅲ)ions from aqueous solution[J].Colloids&Surfaces A:Physicochemical&Engineering Aspects,2016,509:550-563.
[13] MA Ying,LIU Wujun,ZHANG Nan,et al. Polyethylenimine modified biochar adsorbent for hexavalent chromium removal from the aqueous solution[J]. Bioresource Technology,2014,169(5):403-408.
[14] WANG Shujuan,GUO Wei,GAO Fan,et al. Characterization and Pb(Ⅱ)removal potential of corn straw-and municipal sludgederived biochars[J]. Royal Society Open Science,2017. doi:10. 1098/rsos. 170402.
[15] YANTASEE W,LIN Yuehe,ALFORRDK L,et al. Electrophilic aromatic substitutions of amine and sulfonate onto fine-grained activated carbon for aqueous-phase metal ion removal[J].Separation Science Technology,2004,39:3263-3279.
[16] HUANG S,CHEN D. Rapid removal of heavy metal cations and anions from aqueoussolutions by an amino-functionalized magnetic nano-adsorbent[J].Journal of Hazardous Materials,2009,163(1):174-179.
[17] LU Huanliang,ZHANG Weihua,YANG Yuxi.Relative distribution of Pb2+sorption mechanisms by sludge-derived biochar[J]. Water Research,2012,46:854-862.
[18] HUANG Xixian,LIU Yunguo,LIU Shaobo,et al.Effective removal of Cr(Ⅵ)usingβ-cyclodextrin-chitosan modified biochars with adsorption/reduction bifuctional roles[J]. Rsc Advances,2015,6(1):94-104.
[19] DING Wenchuan,DONG Xiaoling,MANDU I I. Pyrolytic temperatures impact lead sorption mechanisms by bagasse biochars[J].Chemosphere,2014,105:68-74.
[20] CHUN Yuan,SHENG Guanyao,CHIOUC T,et al.Compositions and sorptive properties of crop residue-derived chars[J].Environmental Science&Technology,2004,38(17):4649-4655.
[21] SCHMIDT M W I,NOAKC A G. Black carbon in soils and sediments:analysis, distribution, implications, and current challenges[J]. Global Biogeochemical Cycles,2000,14(3):777-793.
[22]马亚红,黄婉婷,刁开盛,等.氨化松香基交联聚和树脂对水中诺氟沙星的吸附性能[J].环境科学,2018,39(1):161-169.MA Yahong,HUANG Wanting,DIAO Kaisheng,et al.Evaluation of performance of an aminated rosin-based resin for adsorption of norfloxacin from aqueous solutions[J]. Environmental Science,2018,39(1):161-169.
[23] LAU A Y T,TSHANG D C W,GRAHAM N J D,et al. Surfacemodified biochar in a bioretention system for escherichia coli removal from stormwater[J].Chemosphere,2016,169:89-98.
[24] LIU Shaobo,HUANG Binyan,CHA Liyuan,et al.Enhancement of As(Ⅴ)adsorption from aqueous solution by a magnetic chitosan/biochar composite[J].Rsc Advance,2017,7:10891-10900.
[25] HO Y S,MCKAY G. Pseudo-second order model for sorption processes[J].Process Biochemistry,1999,34(5):451-465.
[26] GONDHALEKAR S C,SHUKLAS R. Equilibrium and kinetics study of Uranium(Ⅵ)from aqueous solution by citrus limetta,peels[J]. Journal of Radioanalytical&Nuclear Chemistry,2014,302(1):451-457.
[27] NASSAR N N. Rapid removal and recovery of Pb(Ⅱ)from wastewater by magnetic nano adsorbents[J]. Journal of Hazardous Materials,2010,184(1/2/3):538-546.
[28] LING Lili,LIU Wujun,ZHANG Shun,et al. Magnesium oxide embedded nitrogen self-doped biochar composites:fast and highefficiency adsorption of heavy metals in an aqueous solution[J].Environmental Science&Technology,2017,51(17):10081-10089.
[29] OYEWO O A,ONYANGO M S,WOLKERSDORFER C.Application of banana peels nanosorbent for the removal of radioactive minerals from real mine water[J]. Journal of Environmental Radioactivity,2016,164:369-376.
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