纳米零价镍去除溶液中U(VI)的研究
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摘要
采用液相还原法制备纳米零价镍,并用来去除溶液中的U(VI)。通过SEM、EDS技术表征反应前后材料的形貌,从微观角度分析纳米零价镍去除溶液中U(VI)的机理,并进行了热力学分析。结果表明,纳米零价镍对溶液中U(VI)有良好的去除效果,在室温下,pH=4.0、接触时间60min、固液比0.3g/L和初始浓度50mg/L时,U(VI)的去除率和去除量分别达到了98.44%和182.372mg/g。新制备的纳米零价镍呈明显的球状,颗粒较为分散且粒径较均匀,反应后,材料表面形貌发生变化,呈不规则碎片堆积、粒径变大,且材料中出现了铀元素。热力学研究结果表明,该反应是自发吸热反应,同时也是不可逆的熵增反应。
Nano-zero-valent nickel was prepared by liquid-phase reduction method and used to remove U(VI)from aqueous solution. Micro-morphologies of the materials before and after reaction were characterized by SEM and EDS.Removal mechanism was studied based on thermodynamics.The results show that nano-zero-valent nickel has good removal effect on U(VI)from aqueous solution.Removal rate and capacity of U(VI)is 98.44% and 182.372 mg/g respectively under the conditions including room temperature,pH value of 4.0,contact time of 60 min,ratio of solid to liquid of 0.3 g/L,and initial concentration of 50 mg/L.Particle size of nano-zero-valent nickel is obviously spherical with uniform dispersion.After reaction,surface morphology of the material change to irregular fragments accumulation and particle sizes become larger,and U elements appear in the material.Thermodynamic studies show that the reaction is spontaneous endothermic and irreversible with increasing entropy.
Nano-zero-valent nickel was prepared by liquid-phase reduction method and used to remove U(VI)from aqueous solution. Micro-morphologies of the materials before and after reaction were characterized by SEM and EDS.Removal mechanism was studied based on thermodynamics.The results show that nano-zero-valent nickel has good removal effect on U(VI)from aqueous solution.Removal rate and capacity of U(VI)is 98.44% and 182.372 mg/g respectively under the conditions including room temperature,pH value of 4.0,contact time of 60 min,ratio of solid to liquid of 0.3 g/L,and initial concentration of 50 mg/L.Particle size of nano-zero-valent nickel is obviously spherical with uniform dispersion.After reaction,surface morphology of the material change to irregular fragments accumulation and particle sizes become larger,and U elements appear in the material.Thermodynamic studies show that the reaction is spontaneous endothermic and irreversible with increasing entropy.
引文
[1]刘媛媛,魏强林,高柏,等.放射性核素在不同介质中的迁移规律研究现状及进展[J].有色金属(冶炼部分),2018(6):76-82.
[2]KUMARI N.Extraction studies of uranium into a thirdphase of thorium nitrate employing tributyl phosphate and N,N-dihexyl octanamide as extractants in different diluents[J].Journal Radioanalytical and Nuclear Chemistry,2011,290(3):835-843.
[3]SINGH J,DUTTA P K.Preparation,circular dichroism induced helical conformation and optical property of chitosan acid salt complexes for biomedical applications[J].International Journal of Biological Macromolecules,2009,45(4):384-392.
[4]KUMIRSKA J,WEINHOLD M X,SAUVAGAEU J,et al.Determination of the pattern of acetylation of lowmolecular-weight chitosan used in biomedical applications[J].Journal of Pharmaceutical and Biomedical Analysis,2009,50(4):587-590.
[5]魏广芝,徐乐昌.低浓度含铀废水的处理技术及其研究进展[J].铀矿冶,2007,26(2):90-95.
[6]彭国文.新型功能化吸附剂的制备及其吸附铀的试验研究[D].长沙:中南大学,2014.
[7]ABBASI W A,STREAT M.Adsorption of uranium from aqueous solutions using activated carbon[J].Separation Science and Technology,1994,29(9):1433-1439.
[8]CHENG H X,ZENG K F,YU J T.Adsorption of uranium from aqueous solution by grapheme oxide nanosheets on sepiolite[J].Journal of Radioananlytical and Nuclear Chemistry,2013,298(1):599-603.
[9]张文龙.水热交联壳聚糖基材料的制备及吸附铀的性能研究[D].江西抚州:东华理工大学,2014.
[10]刘文娟,徐伟昌,王宝娥.两种酵母菌吸附铀的对比研究[J].南华大学学报(自然科学版),2003,17(4):68-71.
[11]ZHOU S M,CHEN B H,YUAN L I,et al.Synthesis,characterization,thermodynamic and kinetic investigations on uranium(VI)adsorption using organicinorganic composites:Zirconyl-molybdopyrophosphatetibutyl phosphate[J].Science China Chemistry,2013,56(11):1516-1524.
[12]万小岗,杨胜亚.纳米级零价铁处理含铀废水初步试验研究[J].工业水处理,2012,32(3):42-44.
[13]李小燕,刘义保,张明,等.纳米零价铁去除溶液中的U(VI)的还原动力学研究[J].原子能科学技术,2014,48(1):7-13.
[14]李简萍,罗绮莉,胡嘉欣,等.蒙脱石负载纳米铁镍去除水中的溴酸盐研究[J].广州化工,2017,45(19):78-79.
[15]陈建民.镍基金属纳米复合材料的合成及其催化水合肼分解产氢[D].南昌:江西师范大学,2016.
[16]刘晴晴,李小燕,秦启凤,等.纳米铁镍双金属去除溶液中U(VI)的性能研究[J].有色金属(冶炼部分),2018(7):74-78.
[17]郭金辉,孟凡生,王业耀,等.Cu/Fe和Ni/Fe双金属处理模拟地下水中的铬[J].环境工程学报,2016,10(7):3515-3521.
[18]刘晴晴.纳米Fe~0/Ni~0双金属材料去除溶液中U(Ⅵ)的性能研究[D].南昌:东华理工大学,2018.
[19]XU F Y,DENG S B,XU J,et al.Highly active and stable NiFe bimetal prepared by ball milling for catalytic hydrodechlorination of 4-chlorophenol[J].Environmental Science&Technology,2012,46(8):4576-4582.
[20]LI Q,LIU Y H,CAO X H,et al.Biosorption characteristics of uranium(VI)from aqueous solution by pummelo peel[J].Journal of Radioanalytical&Nuclear Chemistry,2012,293(1):67-73.
[2]KUMARI N.Extraction studies of uranium into a thirdphase of thorium nitrate employing tributyl phosphate and N,N-dihexyl octanamide as extractants in different diluents[J].Journal Radioanalytical and Nuclear Chemistry,2011,290(3):835-843.
[3]SINGH J,DUTTA P K.Preparation,circular dichroism induced helical conformation and optical property of chitosan acid salt complexes for biomedical applications[J].International Journal of Biological Macromolecules,2009,45(4):384-392.
[4]KUMIRSKA J,WEINHOLD M X,SAUVAGAEU J,et al.Determination of the pattern of acetylation of lowmolecular-weight chitosan used in biomedical applications[J].Journal of Pharmaceutical and Biomedical Analysis,2009,50(4):587-590.
[5]魏广芝,徐乐昌.低浓度含铀废水的处理技术及其研究进展[J].铀矿冶,2007,26(2):90-95.
[6]彭国文.新型功能化吸附剂的制备及其吸附铀的试验研究[D].长沙:中南大学,2014.
[7]ABBASI W A,STREAT M.Adsorption of uranium from aqueous solutions using activated carbon[J].Separation Science and Technology,1994,29(9):1433-1439.
[8]CHENG H X,ZENG K F,YU J T.Adsorption of uranium from aqueous solution by grapheme oxide nanosheets on sepiolite[J].Journal of Radioananlytical and Nuclear Chemistry,2013,298(1):599-603.
[9]张文龙.水热交联壳聚糖基材料的制备及吸附铀的性能研究[D].江西抚州:东华理工大学,2014.
[10]刘文娟,徐伟昌,王宝娥.两种酵母菌吸附铀的对比研究[J].南华大学学报(自然科学版),2003,17(4):68-71.
[11]ZHOU S M,CHEN B H,YUAN L I,et al.Synthesis,characterization,thermodynamic and kinetic investigations on uranium(VI)adsorption using organicinorganic composites:Zirconyl-molybdopyrophosphatetibutyl phosphate[J].Science China Chemistry,2013,56(11):1516-1524.
[12]万小岗,杨胜亚.纳米级零价铁处理含铀废水初步试验研究[J].工业水处理,2012,32(3):42-44.
[13]李小燕,刘义保,张明,等.纳米零价铁去除溶液中的U(VI)的还原动力学研究[J].原子能科学技术,2014,48(1):7-13.
[14]李简萍,罗绮莉,胡嘉欣,等.蒙脱石负载纳米铁镍去除水中的溴酸盐研究[J].广州化工,2017,45(19):78-79.
[15]陈建民.镍基金属纳米复合材料的合成及其催化水合肼分解产氢[D].南昌:江西师范大学,2016.
[16]刘晴晴,李小燕,秦启凤,等.纳米铁镍双金属去除溶液中U(VI)的性能研究[J].有色金属(冶炼部分),2018(7):74-78.
[17]郭金辉,孟凡生,王业耀,等.Cu/Fe和Ni/Fe双金属处理模拟地下水中的铬[J].环境工程学报,2016,10(7):3515-3521.
[18]刘晴晴.纳米Fe~0/Ni~0双金属材料去除溶液中U(Ⅵ)的性能研究[D].南昌:东华理工大学,2018.
[19]XU F Y,DENG S B,XU J,et al.Highly active and stable NiFe bimetal prepared by ball milling for catalytic hydrodechlorination of 4-chlorophenol[J].Environmental Science&Technology,2012,46(8):4576-4582.
[20]LI Q,LIU Y H,CAO X H,et al.Biosorption characteristics of uranium(VI)from aqueous solution by pummelo peel[J].Journal of Radioanalytical&Nuclear Chemistry,2012,293(1):67-73.