基于反冲洗铁泥制备的磁性吸附剂除砷及再生
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摘要
为了解决除铁锰生物滤池的反冲洗铁泥作为吸附剂使用后难以收集的问题,利用溶剂热法将其制备成为一种磁性材料(magnetic powder adsorbent, MPA),考察其对As(Ⅴ)的吸附特性,结合FTIR表征明确其吸附机制,并探索吸附砷后的MPA最佳再生条件和再生后性能。研究结果表明:根据Langmuir等温吸附模型计算得到MPA在25,35和45℃下对As(Ⅴ)的吸附量分别为8.694,10.005和13.400 mg/g。MPA在吸附过程中发生专性吸附,与As(Ⅴ)形成稳定结合的内层络合物;极碱性溶液能够使吸附的砷发生解吸,以氢氧化钠溶液为再生液,其质量分数为1%时再生效果最好,温度为55℃时最有利于脱附;再生后的MPA吸附速率变快,但最终吸附量降低;3次再生后吸附量能够保持初始吸附量的71.1%,吸附剂可多次再生重复利用,且吸附性能耗竭的吸附剂能够达到直接填埋要求。
To solve the problem that the backwashing iron residuals in the iron and manganese removal are difficult to collect after adsorption as As removal adsorbent, solvothermal method was used to prepare a magnetic powder adsorbent(MPA). Its adsorption performances were studied and its adsorption mechanism for As(V) was investigated and cleared up by FTIR. In addition, optimum regeneration conditions of saturated MPA and performances of regenerated MPA were studied. The results show that the maximum adsorption capacity of MPA for As(V) calculated by Langmuir isotherm equation at 25, 35 and 45 ℃ are 8.694, 10.005 and 13.400 mg/g, respectively. Specific adsorption occurs and MPA forms stable inner complex with As(V). Under extreme alkaline conditions, the adsorbed arsenic can be easily desorbed from MPA. The optimal mass fraction is 1% using NaOH as regenerating solution, and the best temperature for desorption is55 ℃. The adsorption rate of MPA after regeneration becomes faster, but the adsorption capacity decreases. After three regeneration cycles, the final adsorption capacity maintains 71.1% of the initial value. MPA can be reused for many times,and moreover, the exhausted adsorbent can meet the requirements of landfill without any other treatment.
To solve the problem that the backwashing iron residuals in the iron and manganese removal are difficult to collect after adsorption as As removal adsorbent, solvothermal method was used to prepare a magnetic powder adsorbent(MPA). Its adsorption performances were studied and its adsorption mechanism for As(V) was investigated and cleared up by FTIR. In addition, optimum regeneration conditions of saturated MPA and performances of regenerated MPA were studied. The results show that the maximum adsorption capacity of MPA for As(V) calculated by Langmuir isotherm equation at 25, 35 and 45 ℃ are 8.694, 10.005 and 13.400 mg/g, respectively. Specific adsorption occurs and MPA forms stable inner complex with As(V). Under extreme alkaline conditions, the adsorbed arsenic can be easily desorbed from MPA. The optimal mass fraction is 1% using NaOH as regenerating solution, and the best temperature for desorption is55 ℃. The adsorption rate of MPA after regeneration becomes faster, but the adsorption capacity decreases. After three regeneration cycles, the final adsorption capacity maintains 71.1% of the initial value. MPA can be reused for many times,and moreover, the exhausted adsorbent can meet the requirements of landfill without any other treatment.
引文
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[20]PECINI E M,SPRINGER V,BRIGANTE M,et al.Arsenate interaction with the surface of nanomagnetic particles:High adsorption of full release[J].Journal of Environmental Chemical Engineering,2017,5(5):4917-4922.
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[22]董婧.铁锰复合氧化物的制备及除砷性能研究[D].武汉:武汉理工大学资源与环境工程学院,2013:34-44.DONG Jing.Synthesis and arsenic removal on ferruginous manganese composite oxides[D].Wuhan:Wuhan University of Technology.School of Resource and Environmental Engineering,2013:34-44.
[2]SMEDLEY P L,KINNIBURJH D G.A review of the source,behaviour and distribution of arsenic in natural waters[J].Applied Geochemistry.2002,17(5):517-568.
[3]ABEJ N R,GATEA A.A bibliometric analysis of research on arsenic in drinking water during the 1992-2012 period:An outlook to treatment alternatives for arsenic removal[J].Journal of Water Process Engineering,2015,6:105-119.
[4]陈景,张曙,杨项军,等.铁盐絮凝法从阳宗海湖水中除砷研究与现场扩大试验[J].环境科学,2015,36(1):202-208.CHEN Jing,ZHANG Shu,YANG Xiangjun,et al.Arsenic removal by coagulation process and the field expanding experiments for Yangzonghai Lake[J].Environmental Science,2015,36(1):202-208.
[5]JAESHIN K,MARK M B.Modeling a novel ion exchange process for arsenic and nitrate removal[J].Water Research,2004,38(8):2053-2062.
[6]李新,黄显怀,伍昌年,等.饮用水除砷吸附剂的研究进展[J].工业用水与废水,2011,42(4):1-5.LI Xin,HUANG Xianhuai,WU Changnian,et al.Research progress on adsorbent for arsenic removal from drinking water[J].Industrial Water&Wastewater,2011,42(4):1-5.
[7]NGUYEN C M,BANG S,CHO J,et al.Performance and mechanism of arsenic removal from water by a nanofiltration membrane[J].Desalination,2009,245(1/2/3):82-94.
[8]王晓伟,刘文君,李德生,等.单段式和两段式纳滤与反渗透膜除砷对比研究[J].给水排水,2010,36(7):125-132.WANG Xiaowei,LIU Wenjun,LI Desheng,et al.Comparison investigation on arsenic removal with one stage and two-stage nanofiltration&reverse osmosis membranes[J].Water&Wastewater Engineering,2010,36(7):125-132.
[9]BANERJI T,CHAUDHARI S.Arsenic removal from drinking water by electrocoagulation using iron electrodes-an understanding of the process parameters[J].Journal of Environmental Chemical Engineering,2016,4(4,Part A):3990-4000.
[10]LIN Sen,YANG Hongjun,NA Zhiye,et al.A novel biodegradable arsenic adsorbent by immobilization of iron oxyhydroxide(FeOOH)on the root powder of long-root eichhornia crassipes[J].Chemosphere,2018,192(Supplement C):258-266.
[11]高峰,贾永忠,孙进贺,等.锌冶炼废渣浸出液硫化法除砷的研究[J].环境工程学报,2011,5(4):812-814.GAO Feng,JIA Yongzhong,SUN Jinhe,et al.Study on arsenic removal from acid-leaching solution of zinc smelter slag with sulfide precipitation process[J].Chinese Journal of Environmental Engineering,2011,5(4):812-814.
[12]AKIN I,ARSLAN G,TOR A,et al.Arsenic(V)removal from underground water by magnetic nanoparticles synthesized from waste red mud[J].Journal of Hazardous Materials,2012,235-236(Supplement C):62-68.
[13]曾辉平,赵运新,吕育锋,等.除铁除锰水厂反冲洗泥吸附除砷[J].哈尔滨工业大学学报,2018,50(2):19-26.ZENG Huiping,ZHAO Yunxin,LüYufeng,et al.Arsenic adsorption behaviors of backwash sludge from water works for iron and manganese removal[J].Journal of Harbin Institute of Technology,2018,50(2):19-26.
[14]OCINSKI D,JAVUKOWICZ S I,MAZUR P,et al.Water treatment residuals containing iron and manganese oxides for arsenic removal from water-Characterization of physicochemical properties and adsorption studies[J].Chemical Engineering Journal,2016,294:210-221.
[15]CHEN A S C,SORG T J,WANG Lili,et al.Regeneration of iron-based adsorptive media used for removing arsenic from groundwater[J].Water Research,2015,77:85-97.
[16]刘振中,邓慧萍.负载铁锰氧化物的活性炭除砷酸盐的性能研究[J].哈尔滨工业大学学报,2010,42(8):1317-1322.LIU Zhenzhong,DENG Huiping.Arsenate removal performance on GAC impregnated with Fe-Mn oxide[J].Journal of Harbin Institute of Technology,2010,42(8):1317-1322.
[17]PEHLIVAN E,TRAN T H,OUEDRAOGO W K I,et al.Removal of As(V)from aqueous solutions by iron coated rice husk[J].Fuel Processing Technology,2013,106(2):511-517.
[18]王献辉.喷雾干燥法制备铁基吸附剂及吸附除砷性能研究[D].长沙:湖南大学化学化工学院,2016:18-25.WANG Xianhui.Preparation of Fe-based adsorbents by spray drying and its arsenic adsorption performances[D].Changsha:Hunan University.College of Chemistry and Chemical Engineering,2016:18-25.
[19]张高生.新型复合吸附剂研制及其净水效能和机理研究[D].北京:中国科学院生态环境研究中心,2007:10-32.ZHANG Gaosheng.Development of novel composite adsorbents for water treatment:effectiveness and mechanisms[D].Beijing:Chinses Academy of Sciences.Research Center for EcoEnvironmental Sciences,2007:10-32.
[20]PECINI E M,SPRINGER V,BRIGANTE M,et al.Arsenate interaction with the surface of nanomagnetic particles:High adsorption of full release[J].Journal of Environmental Chemical Engineering,2017,5(5):4917-4922.
[21]肖静.载铁活性炭吸附剂的制备及除砷机理研究[D].湘潭:湘潭大学化工学院,2013:24-31.XIAO Jing.Research on the preparation of iron-coated activated carbon adsorbent and adsorption mechanisms of arsenic[D].Xiangtan:Xiangtan University.Institute of Chemical Technology,2013:24-31.
[22]董婧.铁锰复合氧化物的制备及除砷性能研究[D].武汉:武汉理工大学资源与环境工程学院,2013:34-44.DONG Jing.Synthesis and arsenic removal on ferruginous manganese composite oxides[D].Wuhan:Wuhan University of Technology.School of Resource and Environmental Engineering,2013:34-44.
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