球形木质素负载纳米零价铁去除溴酸盐的研究
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摘要
以球形氰乙基木质素为原料通过液相还原法制备球形木质素负载纳米零价铁材料(LSAC-Fe),用于去除饮用水中微量的溴酸盐。采用场发射扫描电子显微镜(FESEM)、X射线衍射仪(XRD)、X射线光电子能谱仪(XPS)、氮气吸附法(BET)等对其结构进行表征,并探究了不同条件下LSAC-Fe对BrO_3~-的吸附效果及其热力学吸附和去除机理。研究表明,纳米零价铁可较为均匀地负载在球形木质素上,并且LSAC-Fe具有很高的表面活性;BrO_3~-的去除率随着初始溶液p H值的升高而降低,随着BrO_3~-初始溶液质量浓度的增加而降低;LSAC-Fe对BrO_3~-的吸附过程为吸热过程,升温可促进LSAC-Fe对BrO_3~-的吸附。
In order to remove the tracebromate in drinking water,nanoscale zero-valent iron supported on spherical lignin(LSAC-Fe) was synthesized through liquid-phase reduction method using spherical cyanoethyl lignin as raw material.The LSAC-Fe was characterized by field emission scanning electron microscopy(FESEM),X-ray diffractometer(XRD),X-ray photoelectron spectroscopy(XPS) and nitrogen adsorption(BET).The adsorption effect of LSAC-Fe on BrO_3~- under different conditions was investigated,and the thermodynamic adsorption and removal mechanism were studied.The results showed that the nanoscale zero-valent iron was distributed homogeneously on the spherical lignin,and LSAC-Fe had a high surface activity.The removal percentage of BrO_3~- decreased with the increase of the initial p H of the solution of and the initial concentration of BrO_3~-.The BrO_3~- adsorption process of LSAC-Fe was the endothermic process,and the temperature rise was beneficial to the adsorption of BrO_3~- on LSAC-Fe.
In order to remove the tracebromate in drinking water,nanoscale zero-valent iron supported on spherical lignin(LSAC-Fe) was synthesized through liquid-phase reduction method using spherical cyanoethyl lignin as raw material.The LSAC-Fe was characterized by field emission scanning electron microscopy(FESEM),X-ray diffractometer(XRD),X-ray photoelectron spectroscopy(XPS) and nitrogen adsorption(BET).The adsorption effect of LSAC-Fe on BrO_3~- under different conditions was investigated,and the thermodynamic adsorption and removal mechanism were studied.The results showed that the nanoscale zero-valent iron was distributed homogeneously on the spherical lignin,and LSAC-Fe had a high surface activity.The removal percentage of BrO_3~- decreased with the increase of the initial p H of the solution of and the initial concentration of BrO_3~-.The BrO_3~- adsorption process of LSAC-Fe was the endothermic process,and the temperature rise was beneficial to the adsorption of BrO_3~- on LSAC-Fe.
引文
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[2]Yang H W,Lv M,Yang S X,et al.Ozone depletion and bromate formation of bromide-containing reservoir water in the downstream part of the Yellow River[J].Journal of Tsinghua University:Natural Science,2010(9):1400.杨宏伟,吕淼,杨少霞,等.黄河下游含溴水库水臭氧消耗与溴酸盐生成[J].清华大学学报:自然科学版,2010(9):1400.
[3]Shi Y L,Cai Y Q,Mou S F.Progress in the Determination of Trace Level Bromate in Drinking Water[J].Journal of Instrumental Analysis,2007,26(2):282.史亚利,蔡亚岐,牟世芬.饮用水中痕量溴酸盐分析方法的研究进展[J].分析测试学报,2007,26(2):282.
[4]Zhao Y M,Wan H Q,Xu Z Y.Adsorption and reduction of bromate over carbon nanotubes[J].Journal of Nanjing University:Natural Sciences,2017,53(2):286.赵玉敏,万海勤,许昭怡.碳纳米管吸附还原溴酸盐研究[J].南京大学学报:自然科学版,2017,53(2):286.
[5]Zhang Y Q,Wu Q P,Zhang J M,et al.Study On Adsorption Of Bromate From Water By Granular Activated Carbon[J].Technology of Water Treatment,2014(6):36.张永清,吴清平,张菊梅,等.活性炭对水中溴酸盐吸附性能研究[J].水处理技术,2014(6):36.
[6]Xu Z,Liu H,Li A,et al.Bromate removal by electrochemical reduction at boron-doped diamond electrode[J].Electrochimica Acta,2012,62(1):181.
[7]Westerhoff P.Reduction of Nitrate,Bromate,and Chlorate by Zero Valent Iron(Fe O)[J].Journal of Environmental Engineering,2003,129(1):10.
[8]Sherman M Ponder,John G Darab,Jerome Bucher,et al.Surface Chemistry and Electrochemistry of Supported Zerovalent Iron Nanoparticles in the Remediation of Aqueous Metal Contaminants[J].Chemistry of Materials,2001,13(2):479.
[9]Schrick B,Blough J L,Jones A D,et al.Hydrodechlorination of Trichloroethylene to Hydrocarbons Using Bimetallic Nickel-Iron Nanoparticles[J].Chemistry of Materials,2002,14(14):5140.
[10]Hong S N,Liu M H,Fan J,et al.Research on the Lignin Adsorbents:Actuality and Trend[J].Paper Science&Technology.2004,23(2):38.洪树楠,刘明华,范娟,等.木质素吸附剂研究现状及进展[J].造纸科学与技术,2004,23(2):38.
[11]Jiang T D.Lignin[M].Beijing:Chemical Industry Press,2001:1.蒋挺大.木质素[M].北京:化学工业出版社,2001:1.
[12]Wang J J,Zhang Y F,Chi R A,et al.Adsorption Behavior of Lead Ion on Modified Sodium Lignosulfonate[J].Journal of Wuhan Institute of Technology,2017,39(1):12.王珏珏,张越非,池汝安,等.改性木质素磺酸钠对铅离子的吸附行为研究[J].武汉工程大学学报,2017,39(1):12.
[13]Zhou Y,Bian Q Q,Luo Y J,et al.Adsorption of Aniline on a Modified Alkali Lignin[J].Journal of Anhui Agricultural Sciences,2011,39(25):15554.周艳,边清泉,罗娅君,等.改性碱木质素对苯胺的吸附研究[J].安徽农业科学,2011,39(25):15554.
[14]Miao T B,Chen H,LIU M H.Adsorption Behavior of Methylene Blue on Cyanoethyl Spherical Lignin Adsorbent[J].Transactions of China Pulp and Paper,2015,30(1):40.苗天博,陈葓,刘明华.氰乙基球形木质素吸附剂对亚甲基蓝的吸附行为研究[J].中国造纸学报,2015,30(1):40.
[15]Dale L,Huber Dr.Synthesis,Properties,and Applications of Iron Nanoparticles[J].Small,2005,1(5):482.
[16]Yang Q,Wu X Q,Zhong Y,et al.Removal of Bromate Using Nanoscale Zero-valent Iron Supported on Activated Carbon[J].Journal of Hunan University:Natural Sciences,2013,40(12):97.杨麒,伍秀琼,钟宇,等.活性炭负载纳米零价铁去除溴酸盐的研究[J].湖南大学学报:自然科学版,2013,40(12):97.
[17]Leyva-Ramos R,Fuentes-Rubio L,Guerrero-Coronado R M,et al.Adsorption of trivalent chromium from aqueous solutions onto activated carbon[J].Journal of Chemical Technology&Biotechnology Biotechnology,2010,62(1):64.
[18]Wei L,Wang K,Zhao Q,et al.Kinetics and equilibrium of adsorption of dissolved organic matter fractions from secondary effluent by fly ash[J].Journal of Environmental Sciences,2011,23(7):1057.
[19]Panday K K,Prasad G,Singh V N.Copper(II)removal from aqueous solutions by fly ash[J].Water Research,1985,19(7):869.
[20]Wang W,Jin Z H,Li T L,et al.Preparation of spherical iron nanoclusters in ethanol-water solution for nitrate removal.[J].Chemosphere,2006,65(8):1396.