UV增强Fe~(2+)活化过硫酸氢钾降解罗丹明B
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摘要
文章研究了紫外光(UV)辐射对微量Fe~(2+)活化过硫酸氢钾(PMS)降解罗丹明B(RhB)的增强作用以及其反应机理。考察了初始pH值、Fe~(2+)投加量、PMS初始浓度和RhB初始浓度等参数对UV/Fe~(2+)/PMS体系降解RhB的影响。对反应体系中的活性自由基、水中常见离子和腐殖酸对反应体系的影响以及RhB的矿化情况进行了探究。结果表明,在溶液体系pH值为3、Fe~(2+)投加量为50μmol/L、PMS浓度为500μmol/L的最佳条件下,10 mg/L RhB在体系反应10 min时降解率达到99%。自由基猝灭实验表明了硫酸根自由基和羟基自由基是攻击RhB分子的活性自由基,硫酸根自由基起到主要作用。水体中常见的碳酸氢根离子和腐殖酸在低浓度会促进降解而高浓度则抑制降解,氯离子则抑制降解反应。对TOC进行分析,60 min时RhB的矿化度达到48%。通过评估UV/Fe~(2+)/PMS体系降解RhB,验证了UV辐射对降解反应的增强作用,表明了UV/Fe~(2+)/PMS体系降解RhB的有效性。
In this paper,the enhanced effect of ultraviolet(UV)radiation on the degradation of Rhodamine B(RhB)by trace Fe~(2+)activated potassium persulfate(PMS)and its reaction mechanism were studied.The effects of initial pH value,Fe~(2+)dosage,initial PMS concentration and initial RhB concentration on the degradation of RhB by UV/Fe~(2+)/PMS system were investigated.The influence of reactive free radicals,common ions and humic acids in the reaction system on the reaction system,and the mineralization of RhB have also been investigated.The results showed that the degradation rate of 10mg/L RhB in the reaction system for 10 min under the optimal conditions of pH value of solution 3,Fe~(2+)dosage of 50μmol/L and PMS concentration of 500μmol/L,it can reach 99%.Free radical quenching experiments showed that sulfate radicals and hydroxyl radicals are active radicals that attack RhB molecules,and sulfate radicals play a major role.The common bicarbonate ions and humic acids in water promote degradation at low concentrations and inhibit degradation at high concentrations,while chloride ions inhibit degradation reactions.The analysis of TOC showed that the mineralization degree of RhB reached 48%at 60 min.By evaluating the degradation of RhB by the UV/Fe~(2+)/PMS system,the enhancement effect of UV radiation on the degradation reaction was verified,demonstrating the effectiveness of the UV/Fe~(2+)/PMS system for the degradation of RhB.
In this paper,the enhanced effect of ultraviolet(UV)radiation on the degradation of Rhodamine B(RhB)by trace Fe~(2+)activated potassium persulfate(PMS)and its reaction mechanism were studied.The effects of initial pH value,Fe~(2+)dosage,initial PMS concentration and initial RhB concentration on the degradation of RhB by UV/Fe~(2+)/PMS system were investigated.The influence of reactive free radicals,common ions and humic acids in the reaction system on the reaction system,and the mineralization of RhB have also been investigated.The results showed that the degradation rate of 10mg/L RhB in the reaction system for 10 min under the optimal conditions of pH value of solution 3,Fe~(2+)dosage of 50μmol/L and PMS concentration of 500μmol/L,it can reach 99%.Free radical quenching experiments showed that sulfate radicals and hydroxyl radicals are active radicals that attack RhB molecules,and sulfate radicals play a major role.The common bicarbonate ions and humic acids in water promote degradation at low concentrations and inhibit degradation at high concentrations,while chloride ions inhibit degradation reactions.The analysis of TOC showed that the mineralization degree of RhB reached 48%at 60 min.By evaluating the degradation of RhB by the UV/Fe~(2+)/PMS system,the enhancement effect of UV radiation on the degradation reaction was verified,demonstrating the effectiveness of the UV/Fe~(2+)/PMS system for the degradation of RhB.
引文
[1]尹汉雄,唐玉朝,黄显怀,等.紫外光强化Fe(Ⅱ)-EDTA活化过硫酸盐降解直接耐酸大红4BS[J].环境科学研究, 2017,30(7):1105-1111.Yin Hanxiong, Tang Yuchao, Huang Xianhuai, et al. Decolorization effect of direct fast scarlet 4BS by Fe(Ⅱ)-EDTA activated peroxodisulfate under ultraviolet light[J]. Research of Environmental Science, 2017,30(7):1105-1111.
[2] Guan Y H, Ma J, Ren Y M, et al. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Research, 2013,47(14):5431-5438.
[3]张利朋,王枫亮,陈平,等.亚铁离子活化过硫酸氢钾复合盐降解水溶液中酮洛芬[J].环境工程学报, 2017,11(2):847-851.Zhang Lipeng, Wang Fengliang, Chen Ping, et al. Degradation of ketoprofen in aqueous by peroxymonosulfate activated by ferrous ion[J]. Chinese Journal of Environmental Engineering, 2017,11(2):847-851.
[4]高金龙,马玉琳,孟庆来,等.二价铁活化过硫酸盐降解土壤中十溴联苯醚[J].环境工程学报, 2016,10(12):7339-7343.Gao Jinlong, Ma Yulin, Meng Qinglai, et al. Degradation of decabromodiphenyl ether in soil by sulfate activated with ferrous ions[J]. Chinese Journal of Environmental Engineering, 2016,10(12):7339-7343.
[5] Martínez Costa J I, Rivera Utrilla J, Leyva Ramos R, et al.Individual and simultaneous degradation of the antibiotics sulfamethoxazole and trimethoprim in aqueous solutions by Fenton, Fenton-like and photo-Fenton processes using solar and UV radiations[J]. Journal of Photochemistry and Photobiology A:Chemistry, 2018,360:95-108.
[6] Anipsitakis G P, Dionysiou D D. Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science and Technology, 2004,38(13):3705-3712.
[7] Liu Y, Guo H, Zhang Y, et al. Activation of peroxymonosulfate by BiVO4under visible light for degradation of Rhodamine B[J]. Chemical Physics Letters, 2016,653:101-107.
[8] Rastogi A, Al Abed S R, Dionysiou D D. Sulfate radicalbased ferrous-peroxymonosulfate oxidative system for PCBs degradation in aqueous and sediment systems[J]. Applied Catalysis B:Environmental, 2009,85(3):171-179.
[9]鲁思伽,洪军,祁士华,等. UV/Fenton体系中Fe2+/Fe3+的相互转化规律[J].环境科学学报, 2009,29(6):1258-1262.Lu Sijia, Hong Jun, Qi Shihua, et al. Transform rules between Fe3+/Fe2+in the UV/Fenton system[J]. Acta Scientiae Circumstantiae, 2009,29(6):1258-1262.
[10] Romero A, Santos A, Vicente F, et al. Diuron abatement using activated persulphate:effect of p H, Fe(II)and oxidant dosage[J]. Chemical Engineering Journal, 2010,162(1):257-265.
[11] Stefánsson A. Iron(Ⅲ)hydrolysis and solubility at 25℃[J].Environmental Science and Technology, 2007,41(17):6117-6123.
[12] Tamimi M, Qourzal S, Barka N, et al. Methomyl degradation in aqueous solutions by Fenton's reagent and the photoFenton system[J]. Separation and Purification Technology,2008,61(1):103-108.
[13] Kakavandi B, Babaei A A. Heterogeneous Fenton-like oxidation of petrochemical wastewater using a magnetically separable catalyst(MNPs@C):process optimization, reaction kinetics and degradation mechanisms[J]. Rsc Advances,2016,6(88):84999-85011.
[14] Jonidi Jafari A, Kakavandi B, Jaafarzadeh N, et al. Fentonlike catalytic oxidation of tetracycline by AC@Fe3O4as a heterogeneous persulfate activator:adsorption and degradation studies[J]. Journal of Industrial and Engineering Chemistry, 2017,45:323-333.
[15] Khan J A, He X, Khan H M, et al. Oxidative degradation of atrazine in aqueous solution by UV/H2O2/Fe2+, UV/S2O82-/Fe2+and UV/HSO5-/Fe2+processes:a comparative study[J].Chemical Engineering Journal, 2013,218:376-383.
[16] Cai C, Zhang H, Zhong X, et al. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe–Co/SBA-15 catalyst for the degradation of OrangeⅡin water[J]. Journal of Hazardous Materials, 2015,283:70-79.
[17] Yang Q, Choi H, Al Abed S R, et al. Iron–cobalt mixed oxide nanocatalysts:heterogeneous peroxymonosulfate activation, cobalt leaching, and ferromagnetic properties for environmental applications[J]. Applied Catalysis B:Environmental, 2009,88(3):462-469.
[18] Lucas M S, Peres J A. Decolorization of the azo dye Reactive Black 5 by Fenton and photo-Fenton oxidation[J]. Dyes and Pigments, 2006,71(3):236-244.
[19] Jiang Q, Spehar A M, H?kansson M, et al. Hot electron-induced cathodic electrochemiluminescence of Rhodamine B at disposable oxide-coated aluminum electrodes[J]. Electrochimica Acta, 2006,51(13):2706-2714.
[20]庞娅,罗琨,李雪,等.磁性氮掺石墨烯活化过硫酸钾降解水中亚甲基蓝[J].环境科学学报, 2017,37(11):4100-4108.Pang Ya, Luo Kun, Li Xue, et al. Activation of potassium persulfate by magnetic nitrogen doped graphene used for degradation of methylene blue[J]. Acta Scientiae Circumstantiae, 2017,37(11):4100-4108.
[21]施周,曾寒轩,邓林.钴铁镍三元水滑石催化PMS降解水中刚果红[J].环境工程学报, 2017,11(9):4903-4909.Shi Zhou, Zeng Hanxuan, Deng Lin. Degradation of congo red in water by catalyzing PMS using ternary CoFeNi-hydrotalcite[J]. Chinese Journal of Environmental Engineering, 2017,11(9):4903-4909.
[22] Anipsitakis G P, Stathatos E, Dionysiou D D. Heterogeneous activation of oxone using Co3O4[J]. Journal of Physical Chemistry B, 2005,109(27):13052-13055.
[23] Lutze H V, Kerlin N, Schmidt T C. Sulfate radical-based water treatment in presence of chloride:formation of chlorate, inter-conversion of sulfate radicals into hydroxyl radicals and influence of bicarbonate[J]. Water Research, 2015,72:349-360.
[24]郭佑罗,高乃云,关小红,等.紫外激活过硫酸盐降解水中双氯芬酸钠[J].哈尔滨工业大学学报, 2017,49(8):65-70.Guo Youluo, Gao Naiyun, Guan Xiaohong, et al. Degradation of diclofenac sodium in water by UV activated persulfate[J]. Journal of Harbin Institute of Technology, 2017,49(8):65-70.
[25] Latifoglu A, Gurol M D. The effect of humic acids on nitrobenzene oxidation by ozonation and O3/UV processes[J].Water Research, 2003,37(8):1879-1889.
[26] Natarajan T S, Thomas M, Natarajan K, et al. Study on UVLED/TiO2process for degradation of Rhodamine B dye[J].Chemical Engineering Journal, 2011,169(1):126-134.
[2] Guan Y H, Ma J, Ren Y M, et al. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Research, 2013,47(14):5431-5438.
[3]张利朋,王枫亮,陈平,等.亚铁离子活化过硫酸氢钾复合盐降解水溶液中酮洛芬[J].环境工程学报, 2017,11(2):847-851.Zhang Lipeng, Wang Fengliang, Chen Ping, et al. Degradation of ketoprofen in aqueous by peroxymonosulfate activated by ferrous ion[J]. Chinese Journal of Environmental Engineering, 2017,11(2):847-851.
[4]高金龙,马玉琳,孟庆来,等.二价铁活化过硫酸盐降解土壤中十溴联苯醚[J].环境工程学报, 2016,10(12):7339-7343.Gao Jinlong, Ma Yulin, Meng Qinglai, et al. Degradation of decabromodiphenyl ether in soil by sulfate activated with ferrous ions[J]. Chinese Journal of Environmental Engineering, 2016,10(12):7339-7343.
[5] Martínez Costa J I, Rivera Utrilla J, Leyva Ramos R, et al.Individual and simultaneous degradation of the antibiotics sulfamethoxazole and trimethoprim in aqueous solutions by Fenton, Fenton-like and photo-Fenton processes using solar and UV radiations[J]. Journal of Photochemistry and Photobiology A:Chemistry, 2018,360:95-108.
[6] Anipsitakis G P, Dionysiou D D. Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science and Technology, 2004,38(13):3705-3712.
[7] Liu Y, Guo H, Zhang Y, et al. Activation of peroxymonosulfate by BiVO4under visible light for degradation of Rhodamine B[J]. Chemical Physics Letters, 2016,653:101-107.
[8] Rastogi A, Al Abed S R, Dionysiou D D. Sulfate radicalbased ferrous-peroxymonosulfate oxidative system for PCBs degradation in aqueous and sediment systems[J]. Applied Catalysis B:Environmental, 2009,85(3):171-179.
[9]鲁思伽,洪军,祁士华,等. UV/Fenton体系中Fe2+/Fe3+的相互转化规律[J].环境科学学报, 2009,29(6):1258-1262.Lu Sijia, Hong Jun, Qi Shihua, et al. Transform rules between Fe3+/Fe2+in the UV/Fenton system[J]. Acta Scientiae Circumstantiae, 2009,29(6):1258-1262.
[10] Romero A, Santos A, Vicente F, et al. Diuron abatement using activated persulphate:effect of p H, Fe(II)and oxidant dosage[J]. Chemical Engineering Journal, 2010,162(1):257-265.
[11] Stefánsson A. Iron(Ⅲ)hydrolysis and solubility at 25℃[J].Environmental Science and Technology, 2007,41(17):6117-6123.
[12] Tamimi M, Qourzal S, Barka N, et al. Methomyl degradation in aqueous solutions by Fenton's reagent and the photoFenton system[J]. Separation and Purification Technology,2008,61(1):103-108.
[13] Kakavandi B, Babaei A A. Heterogeneous Fenton-like oxidation of petrochemical wastewater using a magnetically separable catalyst(MNPs@C):process optimization, reaction kinetics and degradation mechanisms[J]. Rsc Advances,2016,6(88):84999-85011.
[14] Jonidi Jafari A, Kakavandi B, Jaafarzadeh N, et al. Fentonlike catalytic oxidation of tetracycline by AC@Fe3O4as a heterogeneous persulfate activator:adsorption and degradation studies[J]. Journal of Industrial and Engineering Chemistry, 2017,45:323-333.
[15] Khan J A, He X, Khan H M, et al. Oxidative degradation of atrazine in aqueous solution by UV/H2O2/Fe2+, UV/S2O82-/Fe2+and UV/HSO5-/Fe2+processes:a comparative study[J].Chemical Engineering Journal, 2013,218:376-383.
[16] Cai C, Zhang H, Zhong X, et al. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe–Co/SBA-15 catalyst for the degradation of OrangeⅡin water[J]. Journal of Hazardous Materials, 2015,283:70-79.
[17] Yang Q, Choi H, Al Abed S R, et al. Iron–cobalt mixed oxide nanocatalysts:heterogeneous peroxymonosulfate activation, cobalt leaching, and ferromagnetic properties for environmental applications[J]. Applied Catalysis B:Environmental, 2009,88(3):462-469.
[18] Lucas M S, Peres J A. Decolorization of the azo dye Reactive Black 5 by Fenton and photo-Fenton oxidation[J]. Dyes and Pigments, 2006,71(3):236-244.
[19] Jiang Q, Spehar A M, H?kansson M, et al. Hot electron-induced cathodic electrochemiluminescence of Rhodamine B at disposable oxide-coated aluminum electrodes[J]. Electrochimica Acta, 2006,51(13):2706-2714.
[20]庞娅,罗琨,李雪,等.磁性氮掺石墨烯活化过硫酸钾降解水中亚甲基蓝[J].环境科学学报, 2017,37(11):4100-4108.Pang Ya, Luo Kun, Li Xue, et al. Activation of potassium persulfate by magnetic nitrogen doped graphene used for degradation of methylene blue[J]. Acta Scientiae Circumstantiae, 2017,37(11):4100-4108.
[21]施周,曾寒轩,邓林.钴铁镍三元水滑石催化PMS降解水中刚果红[J].环境工程学报, 2017,11(9):4903-4909.Shi Zhou, Zeng Hanxuan, Deng Lin. Degradation of congo red in water by catalyzing PMS using ternary CoFeNi-hydrotalcite[J]. Chinese Journal of Environmental Engineering, 2017,11(9):4903-4909.
[22] Anipsitakis G P, Stathatos E, Dionysiou D D. Heterogeneous activation of oxone using Co3O4[J]. Journal of Physical Chemistry B, 2005,109(27):13052-13055.
[23] Lutze H V, Kerlin N, Schmidt T C. Sulfate radical-based water treatment in presence of chloride:formation of chlorate, inter-conversion of sulfate radicals into hydroxyl radicals and influence of bicarbonate[J]. Water Research, 2015,72:349-360.
[24]郭佑罗,高乃云,关小红,等.紫外激活过硫酸盐降解水中双氯芬酸钠[J].哈尔滨工业大学学报, 2017,49(8):65-70.Guo Youluo, Gao Naiyun, Guan Xiaohong, et al. Degradation of diclofenac sodium in water by UV activated persulfate[J]. Journal of Harbin Institute of Technology, 2017,49(8):65-70.
[25] Latifoglu A, Gurol M D. The effect of humic acids on nitrobenzene oxidation by ozonation and O3/UV processes[J].Water Research, 2003,37(8):1879-1889.
[26] Natarajan T S, Thomas M, Natarajan K, et al. Study on UVLED/TiO2process for degradation of Rhodamine B dye[J].Chemical Engineering Journal, 2011,169(1):126-134.