不同挂膜方式成熟滤料去除地下水中As(Ⅲ)研究
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摘要
通过动力学和动态柱实验对比研究了不同挂膜方式成熟滤料去除地下水中As(Ⅲ)效能.并采用SEM-EDS?XRD及FTIR等表征手段对滤料形态和结构进行了分析.结果表明,两种滤料的形貌具有较大差异.采用化学挂膜的滤料去除As(Ⅲ)性能更优.二级动力学模型能较好地模拟两种滤料除As(Ⅲ)动力学过程,自然挂膜滤料和化学挂膜滤料拟合速率常数分别为8.568×10~(-6)和14.248×10~(-6)mg/(g·min).Yan模型对动态柱实验穿透曲线的拟合系数R~2>0.999.通过脱附再生实验,发现0.5mol/L的NaHCO_3作为脱附剂可使滤料有效再生.对比过滤前后滤料的XRD分析结果,滤料结构变化不大,除砷能力稳定.滤料表面铁锰氧化物含量直接影响滤料除As(Ⅲ)性能.两种滤料在除砷过程中均消耗了羟基.本研究为不同方法去除地下水中As(Ⅲ)提供了理论支撑,具有一定工程指导意义.
A comparative study on the kinetics and column experiment of As(Ⅲ) removal from groundwater by mature filter media formed in different ways was conducted. Besides,a variety of characterization methods were used to analyze the morphology and structure of the two film filter media. The results showed that the morphology was quite different. As(Ⅲ) could be removed more effectively by the chemical film filter media. The second-order model was able to simulate the kinetics of As(Ⅲ) removal well. The fitting rate constants of natural and chemical film filter media were 8.568×10~(-6) and 14.248×10~(-6) mg/(g·min), respectively. The Yan model has a fitting regression coefficient of R~2 >0.999 for the dynamic column breakthrough curve. At the same time, the experiment of desorption and regeneration was carried out. It was found that NaHCO_3 as a desorbent could effectively regenerate the filter media. According to the XRD results of the filter media before and after the filtration, the surface structure did not change much, thus the arsenic removal ability is stable. The content of iron and manganese oxides on the surface of film filter media directly affects the arsenic removal performance. Both film filter media consume hydroxyl groups during the arsenic removal process. The research provides theoretical support for the removal of arsenic from groundwater by different methods and has certain engineering guidance.
A comparative study on the kinetics and column experiment of As(Ⅲ) removal from groundwater by mature filter media formed in different ways was conducted. Besides,a variety of characterization methods were used to analyze the morphology and structure of the two film filter media. The results showed that the morphology was quite different. As(Ⅲ) could be removed more effectively by the chemical film filter media. The second-order model was able to simulate the kinetics of As(Ⅲ) removal well. The fitting rate constants of natural and chemical film filter media were 8.568×10~(-6) and 14.248×10~(-6) mg/(g·min), respectively. The Yan model has a fitting regression coefficient of R~2 >0.999 for the dynamic column breakthrough curve. At the same time, the experiment of desorption and regeneration was carried out. It was found that NaHCO_3 as a desorbent could effectively regenerate the filter media. According to the XRD results of the filter media before and after the filtration, the surface structure did not change much, thus the arsenic removal ability is stable. The content of iron and manganese oxides on the surface of film filter media directly affects the arsenic removal performance. Both film filter media consume hydroxyl groups during the arsenic removal process. The research provides theoretical support for the removal of arsenic from groundwater by different methods and has certain engineering guidance.
引文
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[2]曾辉平,尹灿,李冬,等.基于铁锰泥的除砷吸附剂性能比较及吸附机理[J].中国环境科学,2018,38(9):3373-3379.
[3]Zhu M Q,Paul K W,Kubicki J D,et al.Quantum chemical study of arsenic(III,V)adsorption on Mn-oxides:implications for arsenic(III)oxidation[J].Environmental Science&Technology,2009,43(17):6655-6661.
[4]彭昌军.铁氧化物及铁锰复合氧化物对砷的吸附及其应用研究[D].厦门:厦门大学,2014.
[5]王楠.铁锰氧化物对砷的吸附和氧化特性研究[D].沈阳:沈阳农业大学,2012.
[6]Gude J C,Rietveld L C,Van H D.Fate of low arsenic concentrations during ful-scale aeration and rapid filtration[J].Water Research,2016,88:566-574.
[7]Ociński D,Jacukowicz-Sobala 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.
[8]武俊槟,黄廷林,程亚,等.催化氧化除铁锰氨氮滤池快速启动的影响因素[J].中国环境科学,2017,37(3):1003-1008.
[9]李埜,黄廷林,程亚,等.催化氧化滤池中As(V)与铁?锰?氨氮的协同去除[J].中国给水排水,2017,(23):5-9.
[10]Cheng Y,Huang T,Sun Y,et al.Catalytic oxidation removal of ammonium from groundwater by manganese oxides filter:Performance and mechanisms[J].Chemical Engineering Journal,2017,322:82-89.
[11]Oscarson D W,Huang P M,Defosse C,et al.Oxidative power of Mn(IV)and Fe(III)oxides with respect to As(III)in terrestrial and aquatic environments[J].Nature.1981,291:50-51.
[12]常方方,曲久辉,刘锐平,等.铁锰复合氧化物的制备及其吸附除砷性能[J].环境科学学报,2006,26(11):1769-1774.
[13]Wu Y,Li W,Sparks D L.The effects of iron(II)on the kinetics of arsenic oxidation and sorption on manganese oxides[J].Journal of Colloid&Interface Science,2015,457(1):319-328.
[14]Baktash E,Zaharieva I,Schr?der M,et al.Cyanamide route to calcium-manganese oxide foams for water oxidation[J].Dalton Transactions,2013,42(48):16920-16929.
[15]Limburg J,Szalai V A,Brudvig G W.A mechanistic and structural model for the formation and reactivity of a MnV=O species in photosynthetic water oxidation[J].Journal of the Chemical Society Dalton Transactions,1999,9:1353-1362.
[16]Qi J,Zhang G,Li H.Efficient removal of arsenic from water using a granular adsorbent:Fe-Mn binary oxide impregnated chitosan bead[J].Bioresource Technology,2015,193:243-249.
[17]杨婧.固定床反应器中复合脱氟剂吸附性能的研究[D].武汉:华中科技大学,2011.
[18]Pokhrel D,Viraraghavan T.Arsenic removal in an iron oxide-coated fungal biomass column:analysis of breakthrough curves[J].Bioresource Technology,2008,99(6):2067-2071.
[19]马红梅.微污染饮用水源中砷及几种重金属离子的吸附分离过程研究[D].上海:同济大学,2007.
[20]Cheng Y,Huang T,Shi X,et al.Removal of ammonium ion from water by Na-rich birnessite:Performance and mechanisms[J].Journal of Environmental Sciences,2017,57(7):402-410.
[21]路希鑫.新生态铁锰氧化物和新生态锰氧化物去除水中痕量汞的效能及机理[D].哈尔滨:哈尔滨工业大学,2015.