颗粒无烟煤活性炭去除水体中低浓度磷酸盐研究
|
摘要
为探讨颗粒无烟煤活性炭对水体中低浓度磷酸盐的吸附优化条件、去除效果及其机理,利用小试实验开展不同吸附剂量、温度、吸附时间和pH值等对磷酸盐的吸附影响研究。利用等温吸附、傅里叶变换红外光谱(FTIR)、X射线能谱(XRD)、颗粒Zeta电位、扫描电镜(SEM)表征无烟煤活性炭吸附磷酸盐的特征和机理。结果表明:吸附体系中不同pH值和温度条件对颗粒活性炭吸附磷酸盐的效果影响不同,pH值为6.0时对磷酸盐吸附效果最好,并且在高温条件下有利于活性炭对磷酸盐的吸附。对低浓度磷酸盐[ρ(PO_4~(3-))=2 mg·L~(-1)],颗粒无烟煤活性炭的优化吸附条件为:活性炭用量为10 g·L~(-1)、吸附时间为6 h、pH值为6.0、温度为25℃,磷酸盐的去除率可达80%。颗粒活性炭对磷酸盐的等温吸附符合Langmuir和Freundlich模型,说明对磷酸盐的吸附同时具有物理和化学作用,即磷酸盐不但与活性炭表面官能团之间存在相互吸附作用,且与活性炭上存在的金属离子沉淀作用有关。
In order to clarify the optimum conditions, removal effect and mechanism of low concentration phosphate from aqueous solution by particle anthracite activated carbon(AC). A pilot experiment was conducted to investigate the effects of adsorbent dose, temperature range, adsorption time, and pH on phosphate removal. Characterization and mechanism of phosphate adsorption on anthracite activated carbon by isothermal adsorption, fourier transform infrared spectroscopy(FTIR), X-ray energy spectrum(XRD) and Zeta potential,SEM were studied. The results show that different pH and temperature conditions in the adsorption system have different effects on the adsorption of phosphate on particle activated carbon, and the adsorption effect was the best when pH was 6.0, and it is advantageous to the adsorption of phosphate on activated carbon at high temperature. The optimum adsorption conditions for particle anthracite activated carbon to low concentration phosphate(2 mg·L~(-1)) were as follows:10 g·L~(-1) of anthracite activated carbon, 6 h of adsorption time, 6.0 of the pH, and the removal rate of phosphate was 80%, at 25 ℃. The isothermal adsorption of phosphate on particle activated carbon followed Langmuir and Freundlich models, which showed that the activated carbon had both physical and chemical adsorption on phosphate. So that there was not only mutual adsorption between phosphate and surface functional groups of activated carbon, but also the removal of phosphate was related to the precipitation of metal ions on activated carbon. Therefore, this study provides a basis for the advanced treatment of low concentration phosphate wastewater with anthracite activated carbon.
In order to clarify the optimum conditions, removal effect and mechanism of low concentration phosphate from aqueous solution by particle anthracite activated carbon(AC). A pilot experiment was conducted to investigate the effects of adsorbent dose, temperature range, adsorption time, and pH on phosphate removal. Characterization and mechanism of phosphate adsorption on anthracite activated carbon by isothermal adsorption, fourier transform infrared spectroscopy(FTIR), X-ray energy spectrum(XRD) and Zeta potential,SEM were studied. The results show that different pH and temperature conditions in the adsorption system have different effects on the adsorption of phosphate on particle activated carbon, and the adsorption effect was the best when pH was 6.0, and it is advantageous to the adsorption of phosphate on activated carbon at high temperature. The optimum adsorption conditions for particle anthracite activated carbon to low concentration phosphate(2 mg·L~(-1)) were as follows:10 g·L~(-1) of anthracite activated carbon, 6 h of adsorption time, 6.0 of the pH, and the removal rate of phosphate was 80%, at 25 ℃. The isothermal adsorption of phosphate on particle activated carbon followed Langmuir and Freundlich models, which showed that the activated carbon had both physical and chemical adsorption on phosphate. So that there was not only mutual adsorption between phosphate and surface functional groups of activated carbon, but also the removal of phosphate was related to the precipitation of metal ions on activated carbon. Therefore, this study provides a basis for the advanced treatment of low concentration phosphate wastewater with anthracite activated carbon.
引文
[1] 常会庆,徐晓峰.活性氧化铝去除不同浓度污水中磷的研究[J].水土保持学报,2013,27(4):181-185.[CHANG Hui-qing,XU Xiao-feng.Phosphate Removal From Different Wastewater Concentration by Activate Aluminum Oxide[J].Journal of Soil and Water Conservation,2013,27(4):181-185.]
[2] KRISHNAN K A,HARIDAS A.Removal of Phosphate From Aqueous Solutions and Sewage Using Natural and Surface Modified Coir Pith[J].Journal of Hazardous Materials,2008,152(2):527-535.
[3] 常会庆,徐晓峰,王世华.球形陶粒滤池对城市尾水净化效果研究[J].生态环境学报,2012,21(8):1452-1456.[CHANG Hui-qing,XU Xiao-feng,WANG Shi-hua.Advanced Treatment of City Tail Water by Bio-Ceramic Filter[J].Ecology and Environmental Sciences,2012,21(8):1452-1456.]
[4] ISMAIL Z Z.Kinetic Study for Phosphate Removal From Water by Recycled Date-Palm Wastes as Agricultural By-Products[J].International Journal of Environment Studies,2012,69(1):135-149.
[5] JYOTHI M D,KIRAN K R,RAVINDHRANATH K.Pollution Control in Wastewaters Using New Biosorbents[J].International Journal of Water Resources and Environmental Engineering,2012,4:73-85.
[6] SELVARATNAM T,PEGALLAPATI A K,MONTELYA F,et al.Evaluation of a Thermo-Tolerant Acidophilic Alga,Galdieria Sulphuraria,for Nutrient Removal From Urban Wastewaters[J].Bioresource Technology,2014,156:395-399.
[7] SEO B S,PARK C M,SONG U,et al.Nitrate and Phosphate Removal Potentials of Three Willow Species and a Bald Cypress From Eutrophic Aquatic Environment[J].Landscape and Ecological Engineering,2010,6(2):211-217.
[8] SHI J,PODOLA B,MELKONIAN M.Removal of Nitrogen and Phosphorus From Wastewater Using Microalgae Immobilized on Twin Layers:An Experimental Study[J].Journal of Applied Phycology,2007,19(5):417-423.
[9] YAN Y B,SUN X Y,MA F B,et al.Removal of Phosphate From Wastewater Using Alkaline Residue[J].Journal of Environmental Sciences,2014,26(5):970-980.
[10] AZAM H M,FINNERAN K T.Fe (Ⅲ) Reduction-Mediated Phosphate Removal as Vivianite [Fe3(PO4)28H2O] in Septic System Wastewater[J].Chemosphere,2014,97:1-9.
[11] 吴晓娜,王助贫,谢恩,等.一株反硝化聚磷菌筛选及其接种量对脱氮除磷效应的影响[J].环境工程学报,2018,12(2):544-551.[WU Xiao-na,WANG Zhu-pin,XIE En,et al.Screening of One Strain of Denitrifying Phosphorus Accumulation Bacteria (DPAB) and Inhibitions Effects of Nitrogen-Phosphorus Removal[J].Chinese Journal of Environmental Engineering,2018,12(2):544-551.]
[12] OLADOJA N A,ADELAGUN R O A,OLOLADE I A,et al.Synthesis of Nano-Sized Hydrocalumite From a Gastropod Shell for Aqua System Phosphate Removal[J].Separation and Purification Technology,2014,124(6):■.Adsorption of Methylene Blue Onto Hazelnut Shell:Kinetics,Mechanism and Activation Parameters[J].Journal of Hazardous Materials,2009,164(1):172-181.
[14] NGUYEN T A H,NGO H H,GUO W S,et al.Modification of Agricultural Waste/By-Products for Enhanced Phosphate Removal and Recovery:Potential and Obstacles[J].Bioresource Technology,2014,169:750-762.
[15] WAJIMA T,RAKOVAN J F.Removal Behavior of Phosphate From Aqueous Solution by Calcined Paper Sludge[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2013,435:132-138.
[16] XU K,DENG T,LIU J T,et al.Study on the Phosphate Removal From Aqueous Solution Using Modified Fly Ash[J].Fuel,2010,89(12):3668-3674.
[17] 申战辉,史嘉璐,樊静.负载型纳米Fe/Ni材料同步去除水中硝酸盐/磷酸盐[J].工业水处理,2017,37(5):53-57.[SHEN Zhan-hui,SHI Jia-lu,FAN Jing.Fe/Ni Bimetal Supported Nano-Particle Composite Materials for the Simultaneous Removal of Nitrate/Phosphate From Water[J].Industrial Water Treatment,2017,37(5):53-57.]
[18] CHEN B.Film-Pore Diffusion Modeling and Contact Time Optimization for the Adsorption of Dyestuffs on Pith[J].Chemical Engineering Journal,2001,84(2):77-94.
[19] HO Y S,MCKAY G.Sorption of Dye from Aqueous Solution by Peat[J].Chemical Engineering Journal,1998,70(2):115-124.
[20] LIN X Q,JIN Y Q,WU H L,et al.Removal of PCDD/Fs and PCBs From Flue Gas Using a Pilot Gas Cleaning System[J].Journal of Environmental Sciences,2013,25(9):1833-1840.
[21] RAZVIGOROVA M,BUDINOVA T,PETROV N,et al.Purification of Water by ACs From Apricot Stones,Lignites and Anthracite[J].Water Research,1998,32(7):2135-2139.
[22] AWWAD N S,EL-ZAHHAR A A,FOUDA A M,et al.Removal of Heavy Metal Ions From Ground and Surface Water Samples Using Carbons Derived From Date Pits[J].Journal of Environmental Chemical Engineering,2013,1(3):416-423.
[23] 赵研,郎朗,姜彬慧,等.玉米芯基活性炭吸附去除水中重金属的实验及机理研究[J].东北大学学报(自然科学版),2018,39(3):441-445.[ZHAO Yan,LANG Lang,JIANG Bin-hui,et al.Experiment and Mechanistic Study on Adsorption and Removal of Heavy Metals in Water by Corncob-Based Activated Carbon[J].Journal of Northeastern University(Natural Science),2018,39(3):441-445.]
[24] EMAMI Z,AZIZIAN S.Preparation of Activated Carbon From Date Sphate Using Microwave Irradiation and Investigation of Its Capability for Removal of Dye Pollutant from Aqueous Media[J].Journal of Analytical and Applied Pyrolysis,2014,108:176-184.
[25] ARSLAN G,PEHLIVAN E.Batch Removal of Chromium (Ⅵ) From Aqueous Solution by Turkish Brown Coals[J].Bioresource Technology,2007,98(15):2836-2845.
[26] 常会庆,王浩,徐晓峰.无烟煤活性炭对酸碱性不同染料废水的吸附研究[J].水土保持学报,2014,28(2):276-280.[CHANG Hui-qing,WANG Hao,XU Xiao-feng.Adsorption Studies of Acid and Base Dyes Wastewater on Anthracite Activated Carbon[J].Journal of Soil and Water Conservation,2014,28(2):276-280.]
[27] LU S G,BAI S Q,SHAN H D.Mechanisms of Phosphate Removal From Aqueous Solution by Blast Furnace Slag and Steel Furnace Slag[J].Journal of Zhejiang Unvierstiy(Science A),2008,9(1):125-132.
[28] OGUZ E.Removal of Phosphate From Aqueous Solution With Blast Furnace Slag[J].Journal of Hazardous Materials,2004,114(1/2/3):131-137.
[29] JENKINS D,FERGUSON J F,MENAR A B.Chemical Processes for Phosphate Removal[J].Water Research,1971,5(7):369-389.
[30] 杨欣妍,魏儒平,杨柳燕.污染底泥制备陶粒及除磷潜力研究[J].生态与农村环境学报,2019,35(3):368-376.[YANG Xin-yan,WEI Ru-ping,YANG Liu-yan.Research on Preparing Ceramsite From Polluted River Sediment and the Potential of the Ceramsite on Phosphorus Removal[J].Journal of Ecology and Rural Environment,2019,35(3):368-376.]
[31] 贺凯,卢少勇,金相灿,等.五种填料对磷酸盐的等温吸附-解吸特性[J].农业工程学报,2008,24(8):232-235.[HE Kai,LU Shao-yong,JIN Xiang-can,et al.Adsorption-Desorption Characteristics of Phosphate by Five Kinds of Substrates[J].Transactions of the Chinese Society of Agricultural Engineering,2008,24(8):232-235.]
[32] 赵雪松,胡小贞,卢少勇,等.不同粒径方解石在不同pH值时对磷的等温吸附特征与吸附效果[J].环境科学学报,2008,28(9):1872-1877.[ZHAO Xue-song,HU Xiao-zhen,LU Shao-yong,et al.Phosphorus Sorption by Natural Calcite and the Effects of pH and Grain Size[J].Acta Scientiae Circumstantiae,2008,28(9):1872-1877.]
[33] SAYAG C,SUPPAN S,TRAWCZY■.Effect of Support Activation on the Kinetics of Indole Hydrodenitrogenation Over Mesoporous Carbon Black Composites-Supported Molybdenum Carbide[J].Fuel Processing Technology,2002,77/78:261-267.
[2] KRISHNAN K A,HARIDAS A.Removal of Phosphate From Aqueous Solutions and Sewage Using Natural and Surface Modified Coir Pith[J].Journal of Hazardous Materials,2008,152(2):527-535.
[3] 常会庆,徐晓峰,王世华.球形陶粒滤池对城市尾水净化效果研究[J].生态环境学报,2012,21(8):1452-1456.[CHANG Hui-qing,XU Xiao-feng,WANG Shi-hua.Advanced Treatment of City Tail Water by Bio-Ceramic Filter[J].Ecology and Environmental Sciences,2012,21(8):1452-1456.]
[4] ISMAIL Z Z.Kinetic Study for Phosphate Removal From Water by Recycled Date-Palm Wastes as Agricultural By-Products[J].International Journal of Environment Studies,2012,69(1):135-149.
[5] JYOTHI M D,KIRAN K R,RAVINDHRANATH K.Pollution Control in Wastewaters Using New Biosorbents[J].International Journal of Water Resources and Environmental Engineering,2012,4:73-85.
[6] SELVARATNAM T,PEGALLAPATI A K,MONTELYA F,et al.Evaluation of a Thermo-Tolerant Acidophilic Alga,Galdieria Sulphuraria,for Nutrient Removal From Urban Wastewaters[J].Bioresource Technology,2014,156:395-399.
[7] SEO B S,PARK C M,SONG U,et al.Nitrate and Phosphate Removal Potentials of Three Willow Species and a Bald Cypress From Eutrophic Aquatic Environment[J].Landscape and Ecological Engineering,2010,6(2):211-217.
[8] SHI J,PODOLA B,MELKONIAN M.Removal of Nitrogen and Phosphorus From Wastewater Using Microalgae Immobilized on Twin Layers:An Experimental Study[J].Journal of Applied Phycology,2007,19(5):417-423.
[9] YAN Y B,SUN X Y,MA F B,et al.Removal of Phosphate From Wastewater Using Alkaline Residue[J].Journal of Environmental Sciences,2014,26(5):970-980.
[10] AZAM H M,FINNERAN K T.Fe (Ⅲ) Reduction-Mediated Phosphate Removal as Vivianite [Fe3(PO4)28H2O] in Septic System Wastewater[J].Chemosphere,2014,97:1-9.
[11] 吴晓娜,王助贫,谢恩,等.一株反硝化聚磷菌筛选及其接种量对脱氮除磷效应的影响[J].环境工程学报,2018,12(2):544-551.[WU Xiao-na,WANG Zhu-pin,XIE En,et al.Screening of One Strain of Denitrifying Phosphorus Accumulation Bacteria (DPAB) and Inhibitions Effects of Nitrogen-Phosphorus Removal[J].Chinese Journal of Environmental Engineering,2018,12(2):544-551.]
[12] OLADOJA N A,ADELAGUN R O A,OLOLADE I A,et al.Synthesis of Nano-Sized Hydrocalumite From a Gastropod Shell for Aqua System Phosphate Removal[J].Separation and Purification Technology,2014,124(6):■.Adsorption of Methylene Blue Onto Hazelnut Shell:Kinetics,Mechanism and Activation Parameters[J].Journal of Hazardous Materials,2009,164(1):172-181.
[14] NGUYEN T A H,NGO H H,GUO W S,et al.Modification of Agricultural Waste/By-Products for Enhanced Phosphate Removal and Recovery:Potential and Obstacles[J].Bioresource Technology,2014,169:750-762.
[15] WAJIMA T,RAKOVAN J F.Removal Behavior of Phosphate From Aqueous Solution by Calcined Paper Sludge[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2013,435:132-138.
[16] XU K,DENG T,LIU J T,et al.Study on the Phosphate Removal From Aqueous Solution Using Modified Fly Ash[J].Fuel,2010,89(12):3668-3674.
[17] 申战辉,史嘉璐,樊静.负载型纳米Fe/Ni材料同步去除水中硝酸盐/磷酸盐[J].工业水处理,2017,37(5):53-57.[SHEN Zhan-hui,SHI Jia-lu,FAN Jing.Fe/Ni Bimetal Supported Nano-Particle Composite Materials for the Simultaneous Removal of Nitrate/Phosphate From Water[J].Industrial Water Treatment,2017,37(5):53-57.]
[18] CHEN B.Film-Pore Diffusion Modeling and Contact Time Optimization for the Adsorption of Dyestuffs on Pith[J].Chemical Engineering Journal,2001,84(2):77-94.
[19] HO Y S,MCKAY G.Sorption of Dye from Aqueous Solution by Peat[J].Chemical Engineering Journal,1998,70(2):115-124.
[20] LIN X Q,JIN Y Q,WU H L,et al.Removal of PCDD/Fs and PCBs From Flue Gas Using a Pilot Gas Cleaning System[J].Journal of Environmental Sciences,2013,25(9):1833-1840.
[21] RAZVIGOROVA M,BUDINOVA T,PETROV N,et al.Purification of Water by ACs From Apricot Stones,Lignites and Anthracite[J].Water Research,1998,32(7):2135-2139.
[22] AWWAD N S,EL-ZAHHAR A A,FOUDA A M,et al.Removal of Heavy Metal Ions From Ground and Surface Water Samples Using Carbons Derived From Date Pits[J].Journal of Environmental Chemical Engineering,2013,1(3):416-423.
[23] 赵研,郎朗,姜彬慧,等.玉米芯基活性炭吸附去除水中重金属的实验及机理研究[J].东北大学学报(自然科学版),2018,39(3):441-445.[ZHAO Yan,LANG Lang,JIANG Bin-hui,et al.Experiment and Mechanistic Study on Adsorption and Removal of Heavy Metals in Water by Corncob-Based Activated Carbon[J].Journal of Northeastern University(Natural Science),2018,39(3):441-445.]
[24] EMAMI Z,AZIZIAN S.Preparation of Activated Carbon From Date Sphate Using Microwave Irradiation and Investigation of Its Capability for Removal of Dye Pollutant from Aqueous Media[J].Journal of Analytical and Applied Pyrolysis,2014,108:176-184.
[25] ARSLAN G,PEHLIVAN E.Batch Removal of Chromium (Ⅵ) From Aqueous Solution by Turkish Brown Coals[J].Bioresource Technology,2007,98(15):2836-2845.
[26] 常会庆,王浩,徐晓峰.无烟煤活性炭对酸碱性不同染料废水的吸附研究[J].水土保持学报,2014,28(2):276-280.[CHANG Hui-qing,WANG Hao,XU Xiao-feng.Adsorption Studies of Acid and Base Dyes Wastewater on Anthracite Activated Carbon[J].Journal of Soil and Water Conservation,2014,28(2):276-280.]
[27] LU S G,BAI S Q,SHAN H D.Mechanisms of Phosphate Removal From Aqueous Solution by Blast Furnace Slag and Steel Furnace Slag[J].Journal of Zhejiang Unvierstiy(Science A),2008,9(1):125-132.
[28] OGUZ E.Removal of Phosphate From Aqueous Solution With Blast Furnace Slag[J].Journal of Hazardous Materials,2004,114(1/2/3):131-137.
[29] JENKINS D,FERGUSON J F,MENAR A B.Chemical Processes for Phosphate Removal[J].Water Research,1971,5(7):369-389.
[30] 杨欣妍,魏儒平,杨柳燕.污染底泥制备陶粒及除磷潜力研究[J].生态与农村环境学报,2019,35(3):368-376.[YANG Xin-yan,WEI Ru-ping,YANG Liu-yan.Research on Preparing Ceramsite From Polluted River Sediment and the Potential of the Ceramsite on Phosphorus Removal[J].Journal of Ecology and Rural Environment,2019,35(3):368-376.]
[31] 贺凯,卢少勇,金相灿,等.五种填料对磷酸盐的等温吸附-解吸特性[J].农业工程学报,2008,24(8):232-235.[HE Kai,LU Shao-yong,JIN Xiang-can,et al.Adsorption-Desorption Characteristics of Phosphate by Five Kinds of Substrates[J].Transactions of the Chinese Society of Agricultural Engineering,2008,24(8):232-235.]
[32] 赵雪松,胡小贞,卢少勇,等.不同粒径方解石在不同pH值时对磷的等温吸附特征与吸附效果[J].环境科学学报,2008,28(9):1872-1877.[ZHAO Xue-song,HU Xiao-zhen,LU Shao-yong,et al.Phosphorus Sorption by Natural Calcite and the Effects of pH and Grain Size[J].Acta Scientiae Circumstantiae,2008,28(9):1872-1877.]
[33] SAYAG C,SUPPAN S,TRAWCZY■.Effect of Support Activation on the Kinetics of Indole Hydrodenitrogenation Over Mesoporous Carbon Black Composites-Supported Molybdenum Carbide[J].Fuel Processing Technology,2002,77/78:261-267.