超声波辅助粉煤灰去除水中亚甲基蓝染料的动力学分析
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摘要
为了开发更多的粉煤灰用途,采用粉煤灰去除水中的染料污染物,达到以废治废的目的。采用超声波辅助粉煤灰的方法,以亚甲基蓝染料作为模拟污染物,考察此工艺的可行性,讨论亚甲基蓝的去除效果,分析其动力学。研究结果证明,超声波-粉煤灰联合体系(US-FA体系)具有良好的去除染料污染物的能力,超声波的引入能提高粉煤灰对染料污染物的去除率,协同效应非常明显,粉煤灰投加量0.3、0.5、1.0和2.0 g的情况下,协同因子分别达到1.05、1.32、1.55和2.27。在本实验体系内,经过恒温控制后,超声波的热效应可以忽略,主要通过粉煤灰吸附和羟基自由基降解两大主要途径去除污染物,超声波对去除性能的促进作用主要体现在以下几个方面:一是超声波空化作用产生羟基自由基,超声波和粉煤灰表面相互作用产生更多的羟基自由基;二是超声波能促进粉煤灰表面产生更多的活性位,促进了吸附过程的化学反应步骤,由于粉煤灰对亚甲基蓝的吸附过程以化学反应为控制步骤,所以超声波能大为促进粉煤灰的吸附性能;三是超声波的引入加剧了固液混合,促进污染物向固相表面移动,促进更多的污染物进入到吸附剂颗粒内部,改善了传质。
To develop more use of fly ash, fly ash is used to remove dye contaminants from water to achieve waste treatment. Methylene blue, a kind of dyes, was selected as a model pollutant to investigate the feasibility of the ultrasonic assisted fly ash process(US-FA system). The removal efficiency and the kinetics analysis of this combined system were studied. The experimental results show that the introduction of ultrasonic can improve the removal rate of methylene blue. The synergy effect between fly ash and ultrasound is significant. When fly ash dosage is 0.3, 0.5, 1.0 and 2.0 g, the synergistic factors are 1.05, 1.32, 1.55 and 2.27 respectively. In this experimental scheme, the thermal effect of ultrasonic can be ignored after constant temperature controlling. The pollutant is mainly removed by the adsorption role of fly ash and the degradation role of hydroxyl radicals. The enhancement effect of ultrasound on fly ash is mainly illustrated in aspects as follows:(1) ultrasound cavitation produces hydroxyl radical, and the interaction between ultrasonic wave and fly ash produces more hydroxyl radical,which has strong oxidation ability and non selectivity; therefore the dyes pollutant can be degraded by oxidation of hydroxyl radical.(2) Ultrasonic wave can promote to produce more active sites on the surface of fly ash, therefore ultrasound can greatly promote the adsorption performance of fly ash due to the chemical reaction is the controlling steps of adsorption process of fly ash.(3) Ultrasonic wave aggravates the solid-liquid mixing, promotes the movement of pollutants toward the solid surface, promotes more pollutants to enter into the pores of adsorbent particles, and hence increases the mass transfer of pollutant from liquid phase to solid phase.
To develop more use of fly ash, fly ash is used to remove dye contaminants from water to achieve waste treatment. Methylene blue, a kind of dyes, was selected as a model pollutant to investigate the feasibility of the ultrasonic assisted fly ash process(US-FA system). The removal efficiency and the kinetics analysis of this combined system were studied. The experimental results show that the introduction of ultrasonic can improve the removal rate of methylene blue. The synergy effect between fly ash and ultrasound is significant. When fly ash dosage is 0.3, 0.5, 1.0 and 2.0 g, the synergistic factors are 1.05, 1.32, 1.55 and 2.27 respectively. In this experimental scheme, the thermal effect of ultrasonic can be ignored after constant temperature controlling. The pollutant is mainly removed by the adsorption role of fly ash and the degradation role of hydroxyl radicals. The enhancement effect of ultrasound on fly ash is mainly illustrated in aspects as follows:(1) ultrasound cavitation produces hydroxyl radical, and the interaction between ultrasonic wave and fly ash produces more hydroxyl radical,which has strong oxidation ability and non selectivity; therefore the dyes pollutant can be degraded by oxidation of hydroxyl radical.(2) Ultrasonic wave can promote to produce more active sites on the surface of fly ash, therefore ultrasound can greatly promote the adsorption performance of fly ash due to the chemical reaction is the controlling steps of adsorption process of fly ash.(3) Ultrasonic wave aggravates the solid-liquid mixing, promotes the movement of pollutants toward the solid surface, promotes more pollutants to enter into the pores of adsorbent particles, and hence increases the mass transfer of pollutant from liquid phase to solid phase.
引文
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[13]Li Z,Chen L,Liu S,et al.Characterization of PAHs and PCBs in fly ashes of eighteen coal-fired power plants[J].Aerosol and Air Quality Research,2016,16:3175-3186.
[14]Li Z,Ji Y,Ma H,Zhao P,et al.Characterization of inorganic elements within PM2.5and PM10fractions of fly ashes from coalfired power plants[J].Aerosol and Air Quality Research,2017,17:1105-1116.
[15]Yao Z T,Ji X S,Sarker P K,et al.A comprehensive review on the applications of coal fly ash[J].Earth-Science Reviews,2015,141:105-121.
[16]Saha P,Datta S.Assessment on thermodynamics and kinetics parameters on reduction of methylene blue dye using fly ash[J].Desalin Water Treat,2009,12(1/2/3):531-540.
[17]Sun D,Zhang X,Wu Y,et al.Adsorption of anionic dyes from aqueous solution on fly ash[J].Journal of Hazardous Materials,2010,181:335-342.
[18]Patra G,Barnwal R,Behera S K,et al.Removal of dyes from aqueous solution by sorption with fly ash using a hydrocyclone[J].Journal of Environmental Chemical Engineering,2018,6:5204-5211.
[19]Wang S B,Ma Q,Zhu Z H.Characteristics of coal fly ash and adsorption application[J].Fuel,2008,87:3469-3473.
[20]Hsu T C.Adsorption of an acid dye onto coal fly ash[J].Fuel,2008,87:3040-3045.
[21]Lin J X,Zhan S L,Fang M H,et al.Adsorption of basic dye from aqueous solution onto fly ash[J].Journal of Environmental Management,2008,87:193-200.
[22]Atun G,Ayar N,Kurto?lu A E,et al.A comparison of sorptive removal of anthraquinone and azo dyes using fly ash from single and binary solutions[J].Journal of Hazardous Materials,2019,371:94-107.
[23]Sivalingam S,Sen S.Efficient removal of textile dye using nanosized fly ash derived zeolite-X:kinetics and process optimization study[J].Journal of the Taiwan Institute of Chemical Engineers,2019,96:305-314.
[24]Mushtaq F,Zahid M,Ahmad Bhatti I,et al.Possible applications of coal fly ash in wastewater treatment[J].Journal of Environmental Management,2019,240:27-46.
[25]Eren Z.Ultrasound as a basic and auxiliary process for dye remediation:a review[J].Journal of Environmental Management,2012,104:127-141.
[26]李春喜,王京刚,王子镐,等.超声波技术在污水处理中的应用与研究进展[J].环境污染治理技术与设备,2001,2(2):64-69.Li C X,Wang J G,Wang Z H,et al.Applications and recent advances of ultrasound in waste water treatment[J].Techniques and Equipment for Environmental Pollution Control,2001,2(2):64-69.
[27]Sivalingam S,Sen S.Valorization of coal fly ash into nanozeolite by sonication-assisted hydrothermal method[J].Journal of Environmental Management,2019,235:145-151.
[28]Sivalingam S,Sen S.Rapid ultrasound assisted hydrothermal synthesis of highly pure nanozeolite X from fly ash for efficient treatment of industrial efficient[J].Chemosphere,2018,210:816-823.
[29]Ondarts M,Reinert L,Guittonneau S,et al.Improving the adsorption kinetics of ibuprofen on an activated carbon fabric through ultrasound irradiation:simulation and experimental studies[J].Chemical Engineering Journal,2018,343:163-172.
[30]Wu Y,Han Y B,Tao Y,et al.Ultrasound assisted adsorption and desorption of blueberry anthocyanins using macroporous resins[J].Ultrasonics Sonochemistry,2018,48:311-320.
[31]Hamdaoui O,Naffrechoux E,Tifouti L,et al.Effects of ultrasound on adsorption-desorption of p-chlorophenol on granular activated carbon[J].Ultrasonics Sonochemistry,2003,10:109-114
[32]刘雪粉,俞云良,陆向红,等.超声波应用于吸附/脱附过程的研究进展[J].化工进展,2006,(6):639-645.Liu X F,Yu Y L,Lu X H,et al.Research progress of ultrasound application to adsorption/desorption process[J].Chemical Industry and Engineering Progress,2006,(6):639-645.
[33]Ho Y S.Review of second-order models for adsorption systems[J].Journal of Hazardous Materials,2006,136(3):681-689.
[34]Zhang C L,Zhao F,Wang Y.Thermodynamic and kinetic parameters of ofloxacin adsorption from aqueous solution onto modified coal fly ash[J].Russian Journal of Physical Chemistry A,2012,86(4):653-657.
[35]彭怡,古昌红,傅敏.活性炭改性的研究进展[J].重庆工商大学学报(自然科学版),2007,(6):577-580.Peng Y,Gu C H,Fu M.Research progress in modified activated carbon[J].J.Chongqing Technol.Business Univ.(Nat.Sci.Ed.),2007,(6):577-580.
[36]Heidarinejad Z,Rahmanian O,Fazlzadeh M,et al.Enhancement of methylene blue adsorption onto activated carbon prepared from Date Press Cake by low frequency ultrasound[J].Journal of Molecular Liquids,2018,264:591-599.
[2]Croce R,CinàF,Lombardo A,et al.Aquatic toxicity of several textile dye formulations:acute and chronic assays with Daphnia magna and Raphidocelis subcapitata[J].Ecotoxicology&Environmental Safety,2017,144:79-87.
[3]Vacchi F I,de Souza Vendemiatti J A,da Silva B F,et al.Quantifying the contribution of dyes to the mutagenicity of waters under the influence of textile activities[J].Science of the Total Environment,2017,601/602:230-236.
[4]Jia Q,Song C,Li H,et al.Synthesis of strongly cationic hydrophobic polyquaternium flocculants to enhance removal of water-soluble dyes in wastewater[J].Research on Chemical Intermediates,2017,43(5):3395-3413.
[5]Nidheesh P V,Zhou M,Oturan M A.An overview on the removal of synthetic dyes from water by electrochemical advanced oxidation processes[J].Chemosphere,2018,197:210-227.
[6]Deniz F,Kepekci R A.Bioremediation of contaminated water with unnatural dye using blue-green alga spirulina platensis[J].Environmental Progress&Sustainable Energy,2015,34(5):1414-1419.
[7]BenincáC,Peralta-Zamora P,Tavares C G,et al.Degradation of an azo dye(Ponceau 4R)and treatment of wastewater from a food industry by ozonation[J].Ozone:Science&Engineering,2013,35(4):295-301.
[8]Kavak D.Treatment of dye solutions by DL nanofiltration membrane[J].Desalination&Water Treatment,2017,69:116-122.
[9]Salleh M A M,Mahmoud D K,Karim W A W A,et al.Cationic and anionic dye adsorption by agricultural solid wastes:a comprehensive review[J].Desalination,2011,280(1/2/3):1-13.
[10]Markandeya,Shukla S,Dhiman N.Characterization and adsorption of disperse dyes from wastewater onto cenospheres activated carbon composites[J].Environmental Earth Sciences,2017,76(20):1-12.
[11]Ngulube T,Gumbo J R,Masindi V,et al.An update on synthetic dyes adsorption onto clay based minerals:a state-of-art review[J].Journal of Environmental Management,2017,191:35-57.
[12]王建坤,郭晶,张昊,等.阳离子淀粉染料吸附材料的制备及表征[J].化工学报,2017,68(5):2112-2121.Wang J K,Guo J,Zhang H,et al.Synthesis and characterization of cationic starch dye adsorbing material[J].CIESC Journal,2017,68(5):2112-2121.
[13]Li Z,Chen L,Liu S,et al.Characterization of PAHs and PCBs in fly ashes of eighteen coal-fired power plants[J].Aerosol and Air Quality Research,2016,16:3175-3186.
[14]Li Z,Ji Y,Ma H,Zhao P,et al.Characterization of inorganic elements within PM2.5and PM10fractions of fly ashes from coalfired power plants[J].Aerosol and Air Quality Research,2017,17:1105-1116.
[15]Yao Z T,Ji X S,Sarker P K,et al.A comprehensive review on the applications of coal fly ash[J].Earth-Science Reviews,2015,141:105-121.
[16]Saha P,Datta S.Assessment on thermodynamics and kinetics parameters on reduction of methylene blue dye using fly ash[J].Desalin Water Treat,2009,12(1/2/3):531-540.
[17]Sun D,Zhang X,Wu Y,et al.Adsorption of anionic dyes from aqueous solution on fly ash[J].Journal of Hazardous Materials,2010,181:335-342.
[18]Patra G,Barnwal R,Behera S K,et al.Removal of dyes from aqueous solution by sorption with fly ash using a hydrocyclone[J].Journal of Environmental Chemical Engineering,2018,6:5204-5211.
[19]Wang S B,Ma Q,Zhu Z H.Characteristics of coal fly ash and adsorption application[J].Fuel,2008,87:3469-3473.
[20]Hsu T C.Adsorption of an acid dye onto coal fly ash[J].Fuel,2008,87:3040-3045.
[21]Lin J X,Zhan S L,Fang M H,et al.Adsorption of basic dye from aqueous solution onto fly ash[J].Journal of Environmental Management,2008,87:193-200.
[22]Atun G,Ayar N,Kurto?lu A E,et al.A comparison of sorptive removal of anthraquinone and azo dyes using fly ash from single and binary solutions[J].Journal of Hazardous Materials,2019,371:94-107.
[23]Sivalingam S,Sen S.Efficient removal of textile dye using nanosized fly ash derived zeolite-X:kinetics and process optimization study[J].Journal of the Taiwan Institute of Chemical Engineers,2019,96:305-314.
[24]Mushtaq F,Zahid M,Ahmad Bhatti I,et al.Possible applications of coal fly ash in wastewater treatment[J].Journal of Environmental Management,2019,240:27-46.
[25]Eren Z.Ultrasound as a basic and auxiliary process for dye remediation:a review[J].Journal of Environmental Management,2012,104:127-141.
[26]李春喜,王京刚,王子镐,等.超声波技术在污水处理中的应用与研究进展[J].环境污染治理技术与设备,2001,2(2):64-69.Li C X,Wang J G,Wang Z H,et al.Applications and recent advances of ultrasound in waste water treatment[J].Techniques and Equipment for Environmental Pollution Control,2001,2(2):64-69.
[27]Sivalingam S,Sen S.Valorization of coal fly ash into nanozeolite by sonication-assisted hydrothermal method[J].Journal of Environmental Management,2019,235:145-151.
[28]Sivalingam S,Sen S.Rapid ultrasound assisted hydrothermal synthesis of highly pure nanozeolite X from fly ash for efficient treatment of industrial efficient[J].Chemosphere,2018,210:816-823.
[29]Ondarts M,Reinert L,Guittonneau S,et al.Improving the adsorption kinetics of ibuprofen on an activated carbon fabric through ultrasound irradiation:simulation and experimental studies[J].Chemical Engineering Journal,2018,343:163-172.
[30]Wu Y,Han Y B,Tao Y,et al.Ultrasound assisted adsorption and desorption of blueberry anthocyanins using macroporous resins[J].Ultrasonics Sonochemistry,2018,48:311-320.
[31]Hamdaoui O,Naffrechoux E,Tifouti L,et al.Effects of ultrasound on adsorption-desorption of p-chlorophenol on granular activated carbon[J].Ultrasonics Sonochemistry,2003,10:109-114
[32]刘雪粉,俞云良,陆向红,等.超声波应用于吸附/脱附过程的研究进展[J].化工进展,2006,(6):639-645.Liu X F,Yu Y L,Lu X H,et al.Research progress of ultrasound application to adsorption/desorption process[J].Chemical Industry and Engineering Progress,2006,(6):639-645.
[33]Ho Y S.Review of second-order models for adsorption systems[J].Journal of Hazardous Materials,2006,136(3):681-689.
[34]Zhang C L,Zhao F,Wang Y.Thermodynamic and kinetic parameters of ofloxacin adsorption from aqueous solution onto modified coal fly ash[J].Russian Journal of Physical Chemistry A,2012,86(4):653-657.
[35]彭怡,古昌红,傅敏.活性炭改性的研究进展[J].重庆工商大学学报(自然科学版),2007,(6):577-580.Peng Y,Gu C H,Fu M.Research progress in modified activated carbon[J].J.Chongqing Technol.Business Univ.(Nat.Sci.Ed.),2007,(6):577-580.
[36]Heidarinejad Z,Rahmanian O,Fazlzadeh M,et al.Enhancement of methylene blue adsorption onto activated carbon prepared from Date Press Cake by low frequency ultrasound[J].Journal of Molecular Liquids,2018,264:591-599.