磁化夏威夷果壳活性炭制备及对U(Ⅵ)吸附机理研究
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摘要
实验选用KOH、Fe_3O_4纳米粒子制备磁性夏威夷果壳活性炭,并从磁化活性炭(M-AC)的改性机理、除铀(U)机理、最佳使用条件对磁性夏威夷果壳活性炭除U进行分析。结果表明:磁性活性炭在pH为5时对U去除效率最好,反应140 min后达到吸附平衡,最大吸附量为9.63 mg·g~(-1),去除率可达94.6%。同时实验制备的M-AC在循环实验5次后对U(Ⅵ)去除率仍能达到91%,具有明显的磁选回收再利用能力。吸附等温模型表明吸附过程为单层吸附和多层吸附并存,热力学分析显示吸附过程属于吸热反应,动力学拟合结果则说明吸附过程以化学吸附为主,物理吸附为辅。SEM-EDS、FT-IR、XPS等表征结果进一步说明,由于M-AC在制备、活化过程中增加了醚基、羰基、羧基含量,同时比表面积上升,使得对U(Ⅵ)吸附的有效吸附面积和吸附官能团位点显著增加,提高了普通生物炭的吸附能力。磁性夏威夷果壳活性炭的制备与吸附研究,对于果壳等废料应用提供一种新的思路。
In this research, KOH and Fe_3 O_4 nanoparticles were used to prepare magnetic active carbon from Hawaii nutshell,the modified mechanism of magnetized activated carbon(M-AC),the mechanism of removing uranium and the best use condition were analyzed. The results show that the removal efficiency of u is the best when pH is 5,the adsorption equilibrium is reached after 140 min reaction,the maximum adsorption amount is 9.63 mg·g~(-1),the removal rate can reach 94.6%. At the same time,the removal rate of U(Ⅵ)by MAC can reach 91% after 5 cycles,and the M-AC has obvious ability of magnetic separation recovery and reuse. The adsorption isotherm model shows that the adsorption process consists of both single-layer adsorption and multi-layer adsorption. thermodynamic analysis shows that the adsorption process is an endothermic reaction. The results of SEM-EDS,FT-IR and XPS showed that the content of ether group,carbonyl group and carboxyl group increased and the specific surface area increased during the preparation and activation of M-AC The effective adsorption area and adsorption functional group sites of U(Ⅵ)were increased significantly,and the adsorption capacity of common biochar was improved. The study on the preparation and adsorption of Magnetic Hawaii nutshell activated carbon provides a new idea for the application of waste materials such as Shell.
In this research, KOH and Fe_3 O_4 nanoparticles were used to prepare magnetic active carbon from Hawaii nutshell,the modified mechanism of magnetized activated carbon(M-AC),the mechanism of removing uranium and the best use condition were analyzed. The results show that the removal efficiency of u is the best when pH is 5,the adsorption equilibrium is reached after 140 min reaction,the maximum adsorption amount is 9.63 mg·g~(-1),the removal rate can reach 94.6%. At the same time,the removal rate of U(Ⅵ)by MAC can reach 91% after 5 cycles,and the M-AC has obvious ability of magnetic separation recovery and reuse. The adsorption isotherm model shows that the adsorption process consists of both single-layer adsorption and multi-layer adsorption. thermodynamic analysis shows that the adsorption process is an endothermic reaction. The results of SEM-EDS,FT-IR and XPS showed that the content of ether group,carbonyl group and carboxyl group increased and the specific surface area increased during the preparation and activation of M-AC The effective adsorption area and adsorption functional group sites of U(Ⅵ)were increased significantly,and the adsorption capacity of common biochar was improved. The study on the preparation and adsorption of Magnetic Hawaii nutshell activated carbon provides a new idea for the application of waste materials such as Shell.
引文
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[24]Gu B,Liang L,Dickey M J,et al.Reductive precipitation of uranium(VI)by zero valent iron[J].Environmental Science and Technology,1998,32(21):3366-3373.
[25]Yi Z J,Yao J,Kuang Y F,et al.Uptake of hexavalent uranium from aqueous solutions using coconut husk activated carbon[J].Desalination and Water Treatment,2014,8(3):2016-2019.
[2]Bazyka D A,Prysyazhnyuk A Y,Romanenko A Y,et al.Cancer incidence and nuclear facilities in Ukraine:A community-based study[J].Exp Oncol,2012,34:116-120.
[3]Brugge D,Lemos D J L,Oldmixon B.Exposure pathways and health effects associated with chemical and radiological toxicity of natural uranium:A review[J].Rev Environ Health,2010,20:177-194.
[4]王淑娟,郭伟,史江红,等.氨基修饰稻壳生物炭对水溶液中铀的吸附动力学特性[J].环境科学研究,2019,32(02):347-355.
[5]Kumari N.Extraction studies of uranium into a third-phase of thorium nitrate employing tributyl phosphateand N,Ndihexyl octanamide as extractants in different diluents[J].J Radioanal Nucl Chem,2011,289(3):835-843.
[6]王胜丹.负载钙生物炭回收水中磷酸盐及其产物对铀(Ⅵ)固定的特性研究[D].广州:广州大学,2018.
[7]Kulkarni P S,Mukhopadhyay S,Bellary M P,et al.Studies on membrane stability and recovery of uranium(VI)from aqueous solutions using a liquid emulsionmembrane process[J].Hydrometallurgy,2002,64(1):49-58.
[8]李仕友,胡忠清,廖建彪,等.高锰酸钾改性生物炭对U(Ⅵ)的吸附特性[J].安全与环境学报,2018,18(02):671-677.
[9]Zhu M J,Liu R P,Chai H C,et al.Hazelnut shell activated carbon:a potential adsorbent material for the decontamination of uranium(VI)from aqueous solutions[J].Radioanal Nucl Chem(2016)310:1147-1154.
[10]Yi Z J,Yao J,Kuang F Y,et al,Uptake of hexavalent uranium from aqueous solutions using coconut husk activated carbon[J].Desalination and Water Treatment,2014,977-956.
[11]Yang J,Volesky B.Removal and concentration of uranium by seaweed biosorbent[J].Russ Meteorol Hydro,1999,9:483-492.
[12]Banerjee S,Nigam V,Chattopadhyaya M C.Effective adsorption of anionic dye,Orange G,from aqueous solutions onto activated carbon derived from saw dust by chemical activation with perchloric acid[J].Indian Chemival Society,2018,90:1211-1221.
[13]郭晓慧,康康,王雅君,等.麦秸与木屑热解制备磁性生物炭基材料理化性质研究[J].农业机械学报,2018,49(08):293-300.
[14]Li J L,Li K,Zhang T H,et al.Development of Activated Carbon from Windmill Palm Sheath Fiber by KOH Activation[J].Fibers and Polyme,2016,17(6):880-887.
[15]Duan G J,Liu T H,Wu W S,et al.Adsorption of UO22+from aqueous solution onto copolymers of styrene and maleic anhydride[J].J Radioanal Nucl Chem,2013,295(3):2193-2201.
[16]Hu M Z,Norman J M,Faison B D,et al.Biosorption of uranium by Pseudomonas aeruginosa strain CSU:Characterization and comparison studies[J].Biotechnol Bioeng,1996,51:237-247.
[17]Sar P,Kazy S,D’Souza S.Radionuclide remediation using a bacterial biosorbent[J].Int Biodeterior Biodegrad,2004,54:193-202.
[18]Barkleit A,Foerstendorf H,Li B,et al.Coordination of uranium(VI)with functional groups of bacterial lipopolysaccharide studied by EXAFS and FT-IR spectroscopy[J].Dalton Trans,2011,40:9868-9876.
[19]夏良树,黄欣,曹存存,等.红壤胶体对U(Ⅵ)的吸附性能及机理[J].原子能科学技术,2013,47(10):1692-1699.
[20]冯明明.铀矿山尾矿库区土壤中有机质吸附铀效果与机制研究[D].抚州:东华理工大学,2016.
[21]Han R,Zou W,Wang Y,et al.Removal of U(VI)from aqueous solutions by manganese oxide coated zeolite:discussion of adsorption isotherms and pH effect[J].J Environ Radioact,2007,93:127-143.
[22]Zhang X,Wang J,Li R,et al.Ef fi cient removal of U(VI)from aqueous systems by heattreated carbon microspheres[J].Environ Sci Pollut Res,2013,20:8202-8209.
[23]Yan S,Zhang B H,Zheng Y B,et al.Uranium(VI)removal by nanoscale zero valent iron in anoxic batch systems[J].Environ Scitechnol,2010,44:7783-7789.
[24]Gu B,Liang L,Dickey M J,et al.Reductive precipitation of uranium(VI)by zero valent iron[J].Environmental Science and Technology,1998,32(21):3366-3373.
[25]Yi Z J,Yao J,Kuang Y F,et al.Uptake of hexavalent uranium from aqueous solutions using coconut husk activated carbon[J].Desalination and Water Treatment,2014,8(3):2016-2019.