天然有机物对铁锰复合氧化膜去除氨氮的影响
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摘要
利用中试系统和静态试验,以富里酸为对象,研究天然有机物对石英砂滤料表面负载的铁锰复合氧化膜去除地表水中氨氮的影响。中试结果表明,当富里酸浓度在0～10 mg/L时,富里酸对氨氮的去除没有明显影响,氨氮去除率均高于95. 2%;当富里酸浓度在10～20 mg/L时,氨氮去除率降至65. 4%,甚至出水氨氮超标。静态试验结果表明,氨氮降解过程符合一级反应动力学,相关系数R2> 0. 9,ln(C_0/C_t)与反应时间t有很好的线性关系,随着富里酸浓度的增加,氨氮降解速率k_1值逐渐降低,其中空白的k_1值为0. 012 67 min~(-1),富里酸浓度为5、10和20 mg/L时k_1值分别为空白的78. 6%、63. 4%和57. 6%,即富里酸对氨氮的氧化过程有不利的影响。FTIR光谱分析结果证实了富里酸在铁锰复合氧化膜的表面吸附,且富里酸的羧基离子和铁锰复合氧化膜的表面羟基在吸附过程中起着重要作用。
Iron-manganese co-oxide film coated quartz sands was used to treat surface water,and the effect of natural organic matter( the representative substance was fulvic acid) on the ammonium removal performance was investigated in a pilot-scale filtration system and static experiment. The pilotscale experiment results showed that the removal efficiency of ammonium stabilized over 95. 2% with fulvic acid concentrations ranging from 0 to 10 mg/L,while it fell to 65. 4% and even effluent ammonium concentration exceeded the standard with fulvic acid concentrations ranging from 10 mg/L to 20 mg/L. In static experiment,the degradation of ammonium fitted the first-order reaction kinetics,the related coefficient R~2> 0. 9,ln( C_0/C_t) and the reaction time presented a good linear relation,that was to say,as fulvic acid concentration increasing,the degradation rate of ammonium k_1 value would decrease gradually,among which the blank k_1 was 0. 012 67 min~(-1),while fulvic acid concentration was 5 mg/L,10 mg/L and 20 mg/L,the k_1 values were 78. 6%,63. 4% and 57. 6% of the blank k_1,respectively;fulvic acid played an adverse part in the ammonium oxidation process. FTIR spectra demonstrated the adsorption of fulvic acid on iron-manganese co-oxide film,showing that carboxyl ions in the fulvic acid and the surface hydroxyl of the iron-manganese co-oxide film played an important role in adsorption process.
Iron-manganese co-oxide film coated quartz sands was used to treat surface water,and the effect of natural organic matter( the representative substance was fulvic acid) on the ammonium removal performance was investigated in a pilot-scale filtration system and static experiment. The pilotscale experiment results showed that the removal efficiency of ammonium stabilized over 95. 2% with fulvic acid concentrations ranging from 0 to 10 mg/L,while it fell to 65. 4% and even effluent ammonium concentration exceeded the standard with fulvic acid concentrations ranging from 10 mg/L to 20 mg/L. In static experiment,the degradation of ammonium fitted the first-order reaction kinetics,the related coefficient R~2> 0. 9,ln( C_0/C_t) and the reaction time presented a good linear relation,that was to say,as fulvic acid concentration increasing,the degradation rate of ammonium k_1 value would decrease gradually,among which the blank k_1 was 0. 012 67 min~(-1),while fulvic acid concentration was 5 mg/L,10 mg/L and 20 mg/L,the k_1 values were 78. 6%,63. 4% and 57. 6% of the blank k_1,respectively;fulvic acid played an adverse part in the ammonium oxidation process. FTIR spectra demonstrated the adsorption of fulvic acid on iron-manganese co-oxide film,showing that carboxyl ions in the fulvic acid and the surface hydroxyl of the iron-manganese co-oxide film played an important role in adsorption process.
引文
[1]周怀东,彭文启,杜霞,等.中国地表水水质评价[J].中国水利水电科学研究院学报,2004,2(4):21-30.Zhou Huaidong,Peng Wenqi,Du Xia,et al.Assessment of surface water quality in China[J].Journal of China Institute of Water Resources and Hydropower Research,2004,2(4):21-30(in Chinese).
[2]叶少帆,王志伟,吴志超.微污染水源水处理技术研究进展和对策分析[J].水处理技术,2010,12(6):22-28.Ye Shaofan,Wang Zhiwei,Wu Zhichao.Progress of slightly polluted water resource treatment technology and evaluation on treatment measures[J].Technology of Water Treatment,2010,12(6):22-28(in Chinese).
[3]叶辉,许建华.饮用水中的氨氮问题[J].中国给水排水,2000,16(11):31-34.Ye Hui,Xu Jianhua.The problem of ammonium in drinking water[J].China Water&Wastewater,2000,16(11):31-34(in Chinese).
[4]魏彬,李君,崔营,等.水厂出水加氯消毒的加氯量确定[J].中国给水排水,2010,26(2):86-92.Wei Bin,Li Jun,Cui Ying,et al.Determination of chlorine dosage during chlorination of finished water from waterworks[J].China Water&Wastewater,2010,26(2):86-92(in Chinese).
[5]Enns G M.Neurologic damage and neurocognitive dysfunction in urea cycle disorders[J].Seminars in Pediatric Neurology,2008,15(3):132-139.
[6]何斐,李磊,徐炎华.微污染水源水处理技术研究进展[J].安徽农业科学,2008,36(11):4672-4673.He Fei,Li Lei,Xu Yanhua.Research progress on micropolluted source water treatment[J].Journal of Anhui Agricultural Sciences,2008,36(11):4672-4673(in Chinese).
[7]刘文,吴一蘩.二氧化钛光催化氧化水中天然有机物富里酸[J].净水技术,2010,29(6):66-71.Liu Wen,Wu Yifan.Ti O2photocatalytic oxidation for natural organic matter of fulvic acid in water[J].Water Purification Technology,2010,29(6):66-71(in Chinese).
[8]刘艳芳,王启山,鲁金凤,等.原水天然有机物化学特性与消毒副产物关系[J].水处理技术,2010,36(2):25-28.Liu Yanfang,Wang Qishan,Lu Jinfeng,et al.Chemical characteristic of natural organic matter and relationship with disinfection by-product in drinking water[J].Technology of Water Treatment,2010,36(2):25-28(in Chinese).
[9]林英姿,吕尊敬.饮用水氯消毒副产物的控制研究[J].中国资源综合利用,2017,35(12):62-66.Lin Yingzi,LüZunjing.Studies on the control of chlorine disinfection by-products in drinking water[J].China Resources Comprehensive Utilization,2017,35(12):62-66(in Chinese).
[10]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,2017,33(23):5-9,15.Li Ye,Huang Tinglin,Cheng Ya,et al.Removal of iron,manganese,ammonia nitrogen and arsenic(Ⅴ)by active filter film coating on quartz sands[J].China Water&Wastewater,2017,33(23):5-9,15(in Chinese).
[11]汪洋,黄廷林,文刚,等.地下水中锰对滤料表面氧化膜去除氨氮的影响[J].环境工程学报,2015,9(12):5737-5744.Wang Yang,Huang Tinglin,Wen Gang,et al.Effect of manganese on removal of ammonia from groundwater by co-oxides membrane coated sands[J].Chinese Journal of Environmental Engineering,2015,9(12):5737-5744(in Chinese).
[12]Huang T,Cao X,Wen G,et al.The study on chemical adsorption of dissolved oxygen on naturally formed cooxides filter film in aqueous solution:Combined characterization of XPS and TPD[J].Water Sci Technol,2015,15(2):411-416.
[13]Guo Y,Huang T,Wen G,et al.The simultaneous removal of ammonium and manganese from groundwater by ironmanganese co-oxide filter film:The role of chemical catalytic oxidation for ammonium removal[J].Chem Eng J,2017,308:322-329.
[14]Zhang R,Huang T,Wen G,et al.Phosphate dosing to sustain the ammonium removal activity of an ironmanganese co-oxide filter film at pilot scale:Effects on chemical catalytic oxidation[J].Chem Eng J,2018,334:1186-1194.
[15]Lee C O,Boe-Hansen R,Musovic S,et al.Effects of dynamic operating conditions on nitrification in biological rapid sand filters for drinking water treatment[J].Water Res,2014,64(7):226-236.
[16]李思敏,张建昆,宿程远,等.生物砂滤池去除微污染源水中有机物的试验研究[J].中国给水排水,2006,22(17):57-59.Li Simin,Zhang Jiankun,Su Chengyuan,et al.Study on organic matter removal in micro-polluted source water by biological sand filter[J].China Water&Wastewater,2006,22(17):57-59(in Chinese).
[2]叶少帆,王志伟,吴志超.微污染水源水处理技术研究进展和对策分析[J].水处理技术,2010,12(6):22-28.Ye Shaofan,Wang Zhiwei,Wu Zhichao.Progress of slightly polluted water resource treatment technology and evaluation on treatment measures[J].Technology of Water Treatment,2010,12(6):22-28(in Chinese).
[3]叶辉,许建华.饮用水中的氨氮问题[J].中国给水排水,2000,16(11):31-34.Ye Hui,Xu Jianhua.The problem of ammonium in drinking water[J].China Water&Wastewater,2000,16(11):31-34(in Chinese).
[4]魏彬,李君,崔营,等.水厂出水加氯消毒的加氯量确定[J].中国给水排水,2010,26(2):86-92.Wei Bin,Li Jun,Cui Ying,et al.Determination of chlorine dosage during chlorination of finished water from waterworks[J].China Water&Wastewater,2010,26(2):86-92(in Chinese).
[5]Enns G M.Neurologic damage and neurocognitive dysfunction in urea cycle disorders[J].Seminars in Pediatric Neurology,2008,15(3):132-139.
[6]何斐,李磊,徐炎华.微污染水源水处理技术研究进展[J].安徽农业科学,2008,36(11):4672-4673.He Fei,Li Lei,Xu Yanhua.Research progress on micropolluted source water treatment[J].Journal of Anhui Agricultural Sciences,2008,36(11):4672-4673(in Chinese).
[7]刘文,吴一蘩.二氧化钛光催化氧化水中天然有机物富里酸[J].净水技术,2010,29(6):66-71.Liu Wen,Wu Yifan.Ti O2photocatalytic oxidation for natural organic matter of fulvic acid in water[J].Water Purification Technology,2010,29(6):66-71(in Chinese).
[8]刘艳芳,王启山,鲁金凤,等.原水天然有机物化学特性与消毒副产物关系[J].水处理技术,2010,36(2):25-28.Liu Yanfang,Wang Qishan,Lu Jinfeng,et al.Chemical characteristic of natural organic matter and relationship with disinfection by-product in drinking water[J].Technology of Water Treatment,2010,36(2):25-28(in Chinese).
[9]林英姿,吕尊敬.饮用水氯消毒副产物的控制研究[J].中国资源综合利用,2017,35(12):62-66.Lin Yingzi,LüZunjing.Studies on the control of chlorine disinfection by-products in drinking water[J].China Resources Comprehensive Utilization,2017,35(12):62-66(in Chinese).
[10]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,2017,33(23):5-9,15.Li Ye,Huang Tinglin,Cheng Ya,et al.Removal of iron,manganese,ammonia nitrogen and arsenic(Ⅴ)by active filter film coating on quartz sands[J].China Water&Wastewater,2017,33(23):5-9,15(in Chinese).
[11]汪洋,黄廷林,文刚,等.地下水中锰对滤料表面氧化膜去除氨氮的影响[J].环境工程学报,2015,9(12):5737-5744.Wang Yang,Huang Tinglin,Wen Gang,et al.Effect of manganese on removal of ammonia from groundwater by co-oxides membrane coated sands[J].Chinese Journal of Environmental Engineering,2015,9(12):5737-5744(in Chinese).
[12]Huang T,Cao X,Wen G,et al.The study on chemical adsorption of dissolved oxygen on naturally formed cooxides filter film in aqueous solution:Combined characterization of XPS and TPD[J].Water Sci Technol,2015,15(2):411-416.
[13]Guo Y,Huang T,Wen G,et al.The simultaneous removal of ammonium and manganese from groundwater by ironmanganese co-oxide filter film:The role of chemical catalytic oxidation for ammonium removal[J].Chem Eng J,2017,308:322-329.
[14]Zhang R,Huang T,Wen G,et al.Phosphate dosing to sustain the ammonium removal activity of an ironmanganese co-oxide filter film at pilot scale:Effects on chemical catalytic oxidation[J].Chem Eng J,2018,334:1186-1194.
[15]Lee C O,Boe-Hansen R,Musovic S,et al.Effects of dynamic operating conditions on nitrification in biological rapid sand filters for drinking water treatment[J].Water Res,2014,64(7):226-236.
[16]李思敏,张建昆,宿程远,等.生物砂滤池去除微污染源水中有机物的试验研究[J].中国给水排水,2006,22(17):57-59.Li Simin,Zhang Jiankun,Su Chengyuan,et al.Study on organic matter removal in micro-polluted source water by biological sand filter[J].China Water&Wastewater,2006,22(17):57-59(in Chinese).