载镧活性氧化铝制备及含氟废水除氟因素研究
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摘要
为了提高活性氧化铝除氟性能和拓展矿井水除氟应用领域,采用浸渍焙烧法对活性氧化铝进行改性,制备载镧改性活性氧化铝,并对其制备条件和除氟影响因素进行了试验研究。研究结果表明:当硝酸镧浸渍摩尔浓度0.15 mol/L,焙烧温度350℃,焙烧时间2.5 h,吸附性能达到最佳;载镧活性氧化铝投加质量浓度2.0 g/L,吸附时间120 min,pH值为6.5~7.5,搅拌转速180 r/min时,对12.0mg/L含氟废水的去除率达93%。载镧活性氧化铝吸附除氟过程中浓度对数与反应时间ln C-t曲线服从线性相关,宏观吸附动力学属于一级反应。
In order to improve the fluoride removal performance of activated alumina and expand the application of mine water defluorination,the active alumina adsorbent was modified by lanthanum and the La-loaded active alumina was prepared by impregnation roasting.The preparation conditions were discussed.The adsorption properties were studied in removing fluorine from wastewater. The results show that the adsorption performance is the best when the La( NO_3)3 concentration is 0.15 mol/L,the roasting temperature is 350 ℃ and the roasting time is 2.5 h.The removal rate of 12.0 mg/L fluoride wastewater is 93% when the adsorbent dosage is 2.0 g/L,the adsorption time is 120 min,the pH value is 6.5 ~ 7.5 and the stir speed is 180 r/min.The ln C-t curve in the process of adsorption and fluoride removal with Laloaded activated alumina is basically linearly related and the adsorption belongs to the first-order reaction in macroscopic adsorption kinetics.
In order to improve the fluoride removal performance of activated alumina and expand the application of mine water defluorination,the active alumina adsorbent was modified by lanthanum and the La-loaded active alumina was prepared by impregnation roasting.The preparation conditions were discussed.The adsorption properties were studied in removing fluorine from wastewater. The results show that the adsorption performance is the best when the La( NO_3)3 concentration is 0.15 mol/L,the roasting temperature is 350 ℃ and the roasting time is 2.5 h.The removal rate of 12.0 mg/L fluoride wastewater is 93% when the adsorbent dosage is 2.0 g/L,the adsorption time is 120 min,the pH value is 6.5 ~ 7.5 and the stir speed is 180 r/min.The ln C-t curve in the process of adsorption and fluoride removal with Laloaded activated alumina is basically linearly related and the adsorption belongs to the first-order reaction in macroscopic adsorption kinetics.
引文
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[21]刘琼,郭华明.活化铁锰结核的除氟性能研究[J].环境科学,2009,30(8):2263-2270.LIU Qiong,GUO Huaming.Characteristics of fluoride removal by activated iron-manganese nodules[J].Environmental Science Technology,2009,30(8):2263-2270.
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[23]XU X T.Adsorbtion of fluoride from aqueous solution on magnesialoaded fly ash cenospheres[J].Desalination,2011,272:233-239.
[24]孟范平,李永富,周游,等.EGDE交联的载镧壳聚糖微球对氟离子的静态和动态吸附[J].化工学报,2011,62(11):3192-3200.MENG Fanping,LI Yongfu,ZHOU You,et al.Static and dynamic adsorption of fluoride using La(Ⅲ)-loaded chitosan beads crosslinked with EGDE[J].Journal of chemical Industry and Engineering,2011,62(11):3192-3200.
[25]马刚平,刘振儒,赵春禄.胶吸附氟性能研究[J].中国环境科学,1999,19(4):345-348.MA Gangping,LIU Zhenru,ZHAO Chunlu.Study on the removal of fluride by using lanthanum oxide-coated silica gel[J].China Environmental Science,1999,19(4):345-348.
[2]毛维东,周如禄,郭中权.煤矿矿井水零排放处理技术与应用[J].煤炭科学技术,2017,45(11):205-210.MAO Weidong,ZHOU Rulu,GUO Zhongquan.Zero liquid discharge treatment technology and application for coal mine drainage water[J].Coal Science and Technology,2017,45(11):205-210.
[3]胡涛,李亚云.含氟废水的净化技术研究[J].云南环境科学,2006,25(1):57-59.HU Tao,LI Yayun.Study on purifying technology of fluoride wastewater[J].Yunnan Environment Science,2006,25(1):57-59.
[4]雷绍民,郭振华.氟污染的危害及含氟废水处理技术研究进展[J].金属矿山,2012(4):152-155.LEI Shaomin,GUO Zhenhua.Hazards of fluoride pollution and technical research progress of treating fluoride-containing wastewater[J].Metal Mine,2012(4):152-155.
[5]朱其顺,许光泉.中国地下水氟污染的现状及研究进展[J].环境科学与管理,2009,34(1):42-44.ZHU Qishun,XU Guangquan.The current situation and research progress of ground water fluorine pollution in China[J].Environmental Science and Management,2009,34(1):42-44.
[6]郝阳,孙殿军,魏红联,等.中国大陆地方性氟中毒防治动态与现状分析[J].中国地方病学杂志,2002,21(1):66-71.HAO Yang,SUN Dianjun,WEI Honglian,et al.Analysis on the control trends and present state of endemic fluorosis in china mainland[J].Chinese Journal of Endemiology,2002,21(1):66-71.
[7]赵印英,孟国霞,杨丽霞.山西农村饮水高氟水问题及处理措施分析[J].山西水利科技,2010(3):16-17.ZHAO Yinying,MENG Guoxia,YANG Lixia.On the problems of heavy fluorine compound in Shaoxi’s rural water-drinking and analyzing the treatment measures[J].Shanxi Hydrotechincs,2010(3):16-17.
[8]张金辉,李思,李萍,等.国内外含氟废水吸附处理方法研究进展[J].水处理技术,2013,39(5):7-12.ZHANG Jinhui,LI Si,LI Ping,et al.The review on domestic and overseas adsorption treatment of fluorine wastewater[J].Technology of Water Treatment,2013,39(5):7-12.
[9]WU Daoji,LI Qiumei,YIN Mengmeng,et al.Experiment on Al2O3in removing fluorin of groundwater[J].Acta Scientiarum Naturaliun Universitatis Sunyatseni,2007,46:331-332
[10]周春琼,邓先和,刘海敏,等.吸附法处理含氟水溶液的研究与应用[J].水处理技术,2006,32(1):1-5.ZHOU Chunqiong,DENG Xianhe,LIU Haimin,et al.Treatment of aqueous solution containing fluoride by absorption process[J].Technology of Water Treatment,2006,32(1):1-5.
[11]王东田,尹方平,杨兰.改性活性氧化铝的除氟效能及再生方法研究[J].工业水处理,2010,30(6):55-58.WANG Dongtian,YIN Fangping,YANG Lan.Research on the defluoridation capacity and regeneration of modified activated alumina[J].Industrial Water Treatment,2010,30(6):55-58.
[12]LOUNICI H,BELHOCINEA D,GRIB H,et al.Fluoride removal with electro-activated alumina[J].Desalination,2004,161(1/3):287-293.
[13]SNEHA Jagtap,MAHESH Kumar Yenkie,SERA Das,et al.Synthesis and characterization of lanthanum impregnated chitosan flakes for fluoride removal in water[J].Desalination,2011,273(7):267-275.
[14]刘瑞霞,汤鸿霄.负载镧纤维吸附剂对氟离子的吸附性能[J].环境科学,2000(4):34-37.LIU Ruixia,TANG Hongxiao.Adsorptive properties of fluoride ion on lanthanum-loaded fibrous sorbent[J].Enviromental Scence,2000(4):34-37.
[15]HUANG C,LIU J.Precipitate flotation of fluoride-containing wastewater from a semiconductor manufacturer[J].Water Research,1999,33(16):3403-3412.
[16]KU Y,CHIOU H M.The adsorption of fluoride ion from aqueous solution by activated alumina[J].Water Air Soil Poll,2002,133:349-360.
[17]邓存.活性组分在载体表面的分散状态[J].宁德师专学报:自然科学版,2006,18(4):337-343.DENG Cun.The dispersion of active component on surface of the carrier[J].Journal of Ningde Teachers College:Natural Science,2006,18(4):337-343.
[18]HIEMSTRA T,VAN Riemsdijik W H.Surface structural ion adsorption modeling of competitive binding of oxyanions by metal(hydr)oxides[J].Journal of Colloid and Interface Science,1999,210(1):182-193.
[19]王一凡.Ca-AL-La复合除氟材料的制备及其除氟性能研究[D].武汉:武汉理工大学,2012.
[20]于洋,岳秀萍,刘吉明,等.Mg/Al/Fe型类水滑石焙烧产物吸附去除水中硫酸根离子[J].环境工程学报,2013,7(8):3079-3084.YU Yang,YUE Xiuping,LIU Jiming,et al.Removal of sulfate ions from aqueous solution via adsorption on calcined Mg/Al/Fe hydrotalcite-like compounds[J].Chinese Journal of Environmental Engineering,2013,7(8):3079-3084.
[21]刘琼,郭华明.活化铁锰结核的除氟性能研究[J].环境科学,2009,30(8):2263-2270.LIU Qiong,GUO Huaming.Characteristics of fluoride removal by activated iron-manganese nodules[J].Environmental Science Technology,2009,30(8):2263-2270.
[22]MANIRUDLIAN T S,NOELINE B F,MANOHAR M D.Phosphate removal from wastewaters using a weak anion exchanger prepared from a lignocellulosic residue[J].Environmental Science Technology,2006,40:2740-2745.
[23]XU X T.Adsorbtion of fluoride from aqueous solution on magnesialoaded fly ash cenospheres[J].Desalination,2011,272:233-239.
[24]孟范平,李永富,周游,等.EGDE交联的载镧壳聚糖微球对氟离子的静态和动态吸附[J].化工学报,2011,62(11):3192-3200.MENG Fanping,LI Yongfu,ZHOU You,et al.Static and dynamic adsorption of fluoride using La(Ⅲ)-loaded chitosan beads crosslinked with EGDE[J].Journal of chemical Industry and Engineering,2011,62(11):3192-3200.
[25]马刚平,刘振儒,赵春禄.胶吸附氟性能研究[J].中国环境科学,1999,19(4):345-348.MA Gangping,LIU Zhenru,ZHAO Chunlu.Study on the removal of fluride by using lanthanum oxide-coated silica gel[J].China Environmental Science,1999,19(4):345-348.