热活化过硫酸盐氧化降解水体中泛影酸钠的研究
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摘要
利用热活化过硫酸盐氧化降解水体中的泛影酸钠,主要研究了体系反应温度、氧化剂浓度、溶液初始pH、底物浓度及自然水体组分对降解效果的影响.结果表明,热活化过硫酸盐降解泛影酸钠符合准一级反应动力学模型及遵循阿伦尼乌斯模型,计算得到反应活化能为105.57 kJ·mol~(-1).增加过硫酸盐初始浓度或提高反应温度及降低泛影酸钠初始浓度可以增大泛影酸钠的降解速率常数k(k=0.0062×[K_2S_2O_8]_0,R~2=0.98,[K_2S_2O_8]_0=2～8 mmol·L~(-1);lnk=-12698×1/T+34.91,R~2=0.98,T=325～345 K;k=-1.54×[泛影酸钠]_0+0.064,R~2=0.98).泛影酸钠的降解速率常数k受溶液初始pH影响较小.溶液中Cl~-、HCO~-_3和HA的存在均会抑制泛影酸钠的降解.较低的TOC去除率和产物的检测表明,泛影酸钠降解过程中仅发生苯环侧链的破坏.泛影酸钠的降解途径主要有酰胺键断裂、氨基氧化和脱羧基羟基化.
Thermally activated persulfate oxidation process was applied to degrade sodium diatrizoate in the aqueous solution. The impact factors, such as temperature, the initial concentrations of K_2S_2O_8 and substrate, the initial solution pH and water matrix were investigated. The results show that diatrizoate degradation by thermally activated persulfate oxidation was fitted well with pseudo-first-order mode and Arrhenius equation. The apparent activation energy for this reaction was estimated as 105.57 kJ·mol~(-1). Increasing initial persulfate concentration or temperature and reducing initial substrate concentration significantly increased the apparent rate constant(k) of diatrizoate degradation(k=0.0062×[K_2S_2O_8]_0, R~2=0.98, [K_2S_2O_8]_0=2～8 mmol·L~(-1); lnk=-12698×1/T+34.91, R~2=0.98, T=325～345 K; k=-1.54×[diatrizoate]_0+ 0.064, R~2=0.98), while k was less affected by the initial pH of the solution. The presence of Cl~-, HCO~-_3 and HA in the solution inhibited the degradation of diatrizoate. The low TOC removal rate and formation of organic by-products indicate that the degradation of diatrizoate was incomplete and only its side chain was destructed. The transformation pathways of diatrizoate in the heat-activated persulfate system mainly included amide bond cleavage, amino oxidation and decarboxylation-hydroxylation.
Thermally activated persulfate oxidation process was applied to degrade sodium diatrizoate in the aqueous solution. The impact factors, such as temperature, the initial concentrations of K_2S_2O_8 and substrate, the initial solution pH and water matrix were investigated. The results show that diatrizoate degradation by thermally activated persulfate oxidation was fitted well with pseudo-first-order mode and Arrhenius equation. The apparent activation energy for this reaction was estimated as 105.57 kJ·mol~(-1). Increasing initial persulfate concentration or temperature and reducing initial substrate concentration significantly increased the apparent rate constant(k) of diatrizoate degradation(k=0.0062×[K_2S_2O_8]_0, R~2=0.98, [K_2S_2O_8]_0=2～8 mmol·L~(-1); lnk=-12698×1/T+34.91, R~2=0.98, T=325～345 K; k=-1.54×[diatrizoate]_0+ 0.064, R~2=0.98), while k was less affected by the initial pH of the solution. The presence of Cl~-, HCO~-_3 and HA in the solution inhibited the degradation of diatrizoate. The low TOC removal rate and formation of organic by-products indicate that the degradation of diatrizoate was incomplete and only its side chain was destructed. The transformation pathways of diatrizoate in the heat-activated persulfate system mainly included amide bond cleavage, amino oxidation and decarboxylation-hydroxylation.
引文
Ahmad M,Teel A L,Watts R J.2013.Mechanism of persulfate activation by phenols[J].Environmental Science & Technology,47(11):5864-5871
Azerrad S P,Eversloh C L,Gilboa M,et al.2016.Identification of transformation products during advanced oxidation of diatrizoate:Effect of water matrix and oxidation process[J].Water Research,103:424-434
Del Moro G,Pastore C,Di Iaconi C,et al.2015.Iodinated contrast media electrodegradation:Process performance and degradation pathways[J].Science of the Total Environment,506-507:631-643
Deng J,Shao Y,Gao N,et al.2013.Thermally activated persulfate(TAP) oxidation of antiepileptic drug carbamazepine in water[J].Chemical Engineering Journal,228:765-771
Ens W,Senner F,Gygax B,et al.2014.Development,valisation,and application of a novel LC-MS/MS trace analysis method for the simultaneous quantification of seven iodinated X-ray contrast media and three artificial sweeteners in surface,ground,and drinking water[J].Analytical and Bioanalytical Chemistry,406(12):2789-2798
Eversloh C L,Henning N,Schulz M,et al.2014.Electrochemical treatment of iopromide under conditions of reverse osmosis concentrates-Elucidation of the degradation pathway[J].Water Research,48:237-246
Fang C L,Lou X Y,Huang Y,et al.2017.Monochlorophenols degradation by UV/persulfate is immune to the presence of chloride:Illusion or reality?[J].Chemical Engineering Journal,323:124-133
Gartiser S,Brinker L,Erbe T,et al.1996.Contamination of hospital wastewater with hazardous compounds as defined by 7a WHG[J].Acta Hydrochimica Et Hydrobiologic,24(2):90-97
Ghauch A,Tuqan A M.2012.Oxidation of bisoprolol in heated persulfate/H2O systems:kinetics and products[J].Chemical Engineering Journal,183:162-171
Hu J,Dong H Y,Qu J H,et al.2017.Enhanced degradation of iopamidol by peroxymonosulfate catalyzed by two pipe corrosion products (CuO and d-MnO2) [J].Water Research,112:1-8
Huang Y,Sheng B,Wang Z H,et al.2018.Deciphering the degradation/chlorination mechanisms of maleic acid in the Fe(II)/peroxymonosulfate process:An often overlooked effect of chloride[J].Water Research,145:453-463
Huber M M,Gobel A,Joss A,et al.2005.Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents:A pilot study[J].Environmental Science & Technology,39(11):4290-4299
Jeong J,Jung J,Cooper W J,et al.2010.Degradation mechanisms and kinetic studies for the treatment of X-ray contrast media compounds by advanced oxidation/reduction processes[J].Water Research,44:4391-4398
Kolthoff I M,Miller I K.1951.The chemistry of persulfate.I.The kinetics and mechanism of the decomposition of the persulfate ion in aqueous medium[J].Journal of the American Chemical Society,73:1-30
Liu L,Lin S,Zhang W,et al.2018.Kinetic and mechanistic investigations of the degradation of sulfachloropyridazine in heat-activated persulfate oxidation process[J].Chemical Engineering Journal,346:515-524
Liu Y D,Zhou A G,Gan Y Q,et al.2018.Roles of hydroxyl and sulfate radicals in degradation of trichloroethene by persulfate activated with Fe2+ and zero-valent iron:Insights from carbon isotope fractionation[J].Journal of Hazardous Materials,344:98-103
Lou X Y,Guo Y G,Xiao D X,et al.2013.Rapid dye degradation with reactive oxidants generated by chloride-induced peroxymonosulfate activation[J].Environmental Science & Pollution Research,20:6317-6323
Lutze H V,Bircher S,Rapp I,et al.2015.Degradation of chlorotriazine pesticides by sulfate radicals and the influence of organic matter[J].Environmental Science & Technology,49:1673
Ning B,Graham N J D,Lickiss P D.2009.A comparison of ultrasound-based advanced oxidation processes for the removal of X-ray contrast media[J].Water Science Technology,60:2383-2390
Peng H J,Xu L Y,Zhang W,et al.2017.Different kinds of persulfate activation with base for the oxidation and mechanism of BDE209 in a spiked soil system[J].Science of the Total Environment,574:307-313
Radjenovic J,Petrovic M.2016.Sulfate-mediated electrooxidation of X-ray contrast media on borondoped diamond anode[J].Water Research,94:128-135
Ternes T,Stüber J,Herrmann N,et al.2003.Ozonation:A tool for removal of pharmaceuticals,contrast media and musk fragrances from wastewater[J].Water Research,37:1976-1982
Tian F X,Xu B,Lin Y L,et al.2014.Photodegradation kinetics of iopamidol by UV irradiation and enhanced formation of iodinated disinfection by-products in sequential oxidation processes[J].Water Research,58:198-208
Tian J Y,Wu C W,Yu H R,et al.2018.Applying ultraviolet/persulfate (UV/PS) pre-oxidation for controlling ultrafiltration membrane fouling by natural organic matter (NOM) in surface water[J].Water Research,132:190-199
Velo-Gala I,López-Peňalver J J,Sánchez-Polo M,et al.2012.Ionic X-ray contrast media degradation in aqueous solution induced by gamma radiation[J].Chemical Engineering Journal,195-196:369-376
Velo-Gala I,López-Peňalver J J,Sánchez-Polo M,et al.2014.Comparative study of oxidative degradation of sodium diatrizoate in aqueous solution by H2O2/Fe2+,H2O2/Fe3+,Fe(VI) and UV,H2O2/UV,K2S2O8/UV[J].Chemical Engineering Journal,241:504-512
Wang Q,Lu X H,Cao Y,et al.2017.Degradation of Bisphenol S by heat activated persulfate:Kinetics study,transformation pathways and influences of co-existing chemicals[J].Chemical Engineering Journal,328:236-245
Wang Z H,Feng M,Fang C L,et al.2017a.Both degradation and AOX accumulation are significantly enhanced inUV/peroxymonosulfate/4-chlorophenol/Cl- system:two sides of the same coin?[J].RSC Advance,7:12318-12321
Wang Z H,Ai L Y,Huang Y,et al.2017b.Degradation of azo dye with activated peroxygens:when zero-valent iron meets chloride[J].RSC Advance,7:30941-30948
Wei Z S,Villamena F A,Weavers L K.2017.Kinetics and mechanism of ultrasonic activation of persulfate:An in situ EPR spin trapping study[J].Environmental Science & Technology,51(6):3410-3417
Yang F,Huang Y,Fang C L,et al.2018.Peroxymonosulfate/base process in saline wastewater treatment:The fight between alkalinity and chloride ions[J].Chemosphere,199:84-88
Yang J F,Yang L M,Zhang S B,et al.2017.Degradation of azole fungicide fluconazole in aqueous solution by thermally activated persulfate[J].Chemical Engineering Journal,321:113-122
Yang M,Zhang X.2013.Comparative developmental toxicity of new aromatic halogenated DBPs in a chlorinated saline sewage effluent to the marine polychaete platynereis dumerilii[J].Environmental Science & Technology,47:10868-10876
Ye T,Xu B,Wang Z,Zhang T,et al.2014.Comparison of iodinated trihalomethanes formation during aqueous chlor(am)ination of different iodinated X-ray contrast media compounds in the presence of natural organic matter[J].Water Research,66:390-398
Yen C H,Chen K F,Kao C M,et al.2011.Application of persulfate to remediate petroleum hydrocarbon contaminated soil:feasibility and comparison with common oxidants[J].Journal of Hazardous Materials,186:2097-2102
Zhang Y C,Zhang Q,Dong Z Y,et al.2018.Degradation of acetaminophen with ferrous/copperoxide activate persulfate:Synergism of iron and copper[J].Water Research,146:232-243
Zhou L,Ferronato C,Chovelon J M,et al.2017.Investigations of diatrizoate degradation by photo-activated persulfate[J].Chemical Engineering Journal,311:28-36
Zhou Y,Jiang J,Gao Y,et al.2015.Activation of Peroxymonosulfate by Benzoquinone:A Novel Nonradical Oxidation Process[J].Environmental Science & Technology,49(21):12941-12950
Zhou Y Y,Xiang Y J,He Y Z,et al.2018.Applications and factors influencing of the persulfate-based advanced oxidation processes for the remediation of groundwater and soil contaminated with organic compounds[J].Journal of Hazardous Materials,359:396-407
Zrinyi N,Pham A L.2017.Oxidation of benzoic acid by heat-activated persulfate:Effect of temperature on transformation pathway and product distribution[J].Water Research,120:43-51
Azerrad S P,Eversloh C L,Gilboa M,et al.2016.Identification of transformation products during advanced oxidation of diatrizoate:Effect of water matrix and oxidation process[J].Water Research,103:424-434
Del Moro G,Pastore C,Di Iaconi C,et al.2015.Iodinated contrast media electrodegradation:Process performance and degradation pathways[J].Science of the Total Environment,506-507:631-643
Deng J,Shao Y,Gao N,et al.2013.Thermally activated persulfate(TAP) oxidation of antiepileptic drug carbamazepine in water[J].Chemical Engineering Journal,228:765-771
Ens W,Senner F,Gygax B,et al.2014.Development,valisation,and application of a novel LC-MS/MS trace analysis method for the simultaneous quantification of seven iodinated X-ray contrast media and three artificial sweeteners in surface,ground,and drinking water[J].Analytical and Bioanalytical Chemistry,406(12):2789-2798
Eversloh C L,Henning N,Schulz M,et al.2014.Electrochemical treatment of iopromide under conditions of reverse osmosis concentrates-Elucidation of the degradation pathway[J].Water Research,48:237-246
Fang C L,Lou X Y,Huang Y,et al.2017.Monochlorophenols degradation by UV/persulfate is immune to the presence of chloride:Illusion or reality?[J].Chemical Engineering Journal,323:124-133
Gartiser S,Brinker L,Erbe T,et al.1996.Contamination of hospital wastewater with hazardous compounds as defined by 7a WHG[J].Acta Hydrochimica Et Hydrobiologic,24(2):90-97
Ghauch A,Tuqan A M.2012.Oxidation of bisoprolol in heated persulfate/H2O systems:kinetics and products[J].Chemical Engineering Journal,183:162-171
Hu J,Dong H Y,Qu J H,et al.2017.Enhanced degradation of iopamidol by peroxymonosulfate catalyzed by two pipe corrosion products (CuO and d-MnO2) [J].Water Research,112:1-8
Huang Y,Sheng B,Wang Z H,et al.2018.Deciphering the degradation/chlorination mechanisms of maleic acid in the Fe(II)/peroxymonosulfate process:An often overlooked effect of chloride[J].Water Research,145:453-463
Huber M M,Gobel A,Joss A,et al.2005.Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents:A pilot study[J].Environmental Science & Technology,39(11):4290-4299
Jeong J,Jung J,Cooper W J,et al.2010.Degradation mechanisms and kinetic studies for the treatment of X-ray contrast media compounds by advanced oxidation/reduction processes[J].Water Research,44:4391-4398
Kolthoff I M,Miller I K.1951.The chemistry of persulfate.I.The kinetics and mechanism of the decomposition of the persulfate ion in aqueous medium[J].Journal of the American Chemical Society,73:1-30
Liu L,Lin S,Zhang W,et al.2018.Kinetic and mechanistic investigations of the degradation of sulfachloropyridazine in heat-activated persulfate oxidation process[J].Chemical Engineering Journal,346:515-524
Liu Y D,Zhou A G,Gan Y Q,et al.2018.Roles of hydroxyl and sulfate radicals in degradation of trichloroethene by persulfate activated with Fe2+ and zero-valent iron:Insights from carbon isotope fractionation[J].Journal of Hazardous Materials,344:98-103
Lou X Y,Guo Y G,Xiao D X,et al.2013.Rapid dye degradation with reactive oxidants generated by chloride-induced peroxymonosulfate activation[J].Environmental Science & Pollution Research,20:6317-6323
Lutze H V,Bircher S,Rapp I,et al.2015.Degradation of chlorotriazine pesticides by sulfate radicals and the influence of organic matter[J].Environmental Science & Technology,49:1673
Ning B,Graham N J D,Lickiss P D.2009.A comparison of ultrasound-based advanced oxidation processes for the removal of X-ray contrast media[J].Water Science Technology,60:2383-2390
Peng H J,Xu L Y,Zhang W,et al.2017.Different kinds of persulfate activation with base for the oxidation and mechanism of BDE209 in a spiked soil system[J].Science of the Total Environment,574:307-313
Radjenovic J,Petrovic M.2016.Sulfate-mediated electrooxidation of X-ray contrast media on borondoped diamond anode[J].Water Research,94:128-135
Ternes T,Stüber J,Herrmann N,et al.2003.Ozonation:A tool for removal of pharmaceuticals,contrast media and musk fragrances from wastewater[J].Water Research,37:1976-1982
Tian F X,Xu B,Lin Y L,et al.2014.Photodegradation kinetics of iopamidol by UV irradiation and enhanced formation of iodinated disinfection by-products in sequential oxidation processes[J].Water Research,58:198-208
Tian J Y,Wu C W,Yu H R,et al.2018.Applying ultraviolet/persulfate (UV/PS) pre-oxidation for controlling ultrafiltration membrane fouling by natural organic matter (NOM) in surface water[J].Water Research,132:190-199
Velo-Gala I,López-Peňalver J J,Sánchez-Polo M,et al.2012.Ionic X-ray contrast media degradation in aqueous solution induced by gamma radiation[J].Chemical Engineering Journal,195-196:369-376
Velo-Gala I,López-Peňalver J J,Sánchez-Polo M,et al.2014.Comparative study of oxidative degradation of sodium diatrizoate in aqueous solution by H2O2/Fe2+,H2O2/Fe3+,Fe(VI) and UV,H2O2/UV,K2S2O8/UV[J].Chemical Engineering Journal,241:504-512
Wang Q,Lu X H,Cao Y,et al.2017.Degradation of Bisphenol S by heat activated persulfate:Kinetics study,transformation pathways and influences of co-existing chemicals[J].Chemical Engineering Journal,328:236-245
Wang Z H,Feng M,Fang C L,et al.2017a.Both degradation and AOX accumulation are significantly enhanced inUV/peroxymonosulfate/4-chlorophenol/Cl- system:two sides of the same coin?[J].RSC Advance,7:12318-12321
Wang Z H,Ai L Y,Huang Y,et al.2017b.Degradation of azo dye with activated peroxygens:when zero-valent iron meets chloride[J].RSC Advance,7:30941-30948
Wei Z S,Villamena F A,Weavers L K.2017.Kinetics and mechanism of ultrasonic activation of persulfate:An in situ EPR spin trapping study[J].Environmental Science & Technology,51(6):3410-3417
Yang F,Huang Y,Fang C L,et al.2018.Peroxymonosulfate/base process in saline wastewater treatment:The fight between alkalinity and chloride ions[J].Chemosphere,199:84-88
Yang J F,Yang L M,Zhang S B,et al.2017.Degradation of azole fungicide fluconazole in aqueous solution by thermally activated persulfate[J].Chemical Engineering Journal,321:113-122
Yang M,Zhang X.2013.Comparative developmental toxicity of new aromatic halogenated DBPs in a chlorinated saline sewage effluent to the marine polychaete platynereis dumerilii[J].Environmental Science & Technology,47:10868-10876
Ye T,Xu B,Wang Z,Zhang T,et al.2014.Comparison of iodinated trihalomethanes formation during aqueous chlor(am)ination of different iodinated X-ray contrast media compounds in the presence of natural organic matter[J].Water Research,66:390-398
Yen C H,Chen K F,Kao C M,et al.2011.Application of persulfate to remediate petroleum hydrocarbon contaminated soil:feasibility and comparison with common oxidants[J].Journal of Hazardous Materials,186:2097-2102
Zhang Y C,Zhang Q,Dong Z Y,et al.2018.Degradation of acetaminophen with ferrous/copperoxide activate persulfate:Synergism of iron and copper[J].Water Research,146:232-243
Zhou L,Ferronato C,Chovelon J M,et al.2017.Investigations of diatrizoate degradation by photo-activated persulfate[J].Chemical Engineering Journal,311:28-36
Zhou Y,Jiang J,Gao Y,et al.2015.Activation of Peroxymonosulfate by Benzoquinone:A Novel Nonradical Oxidation Process[J].Environmental Science & Technology,49(21):12941-12950
Zhou Y Y,Xiang Y J,He Y Z,et al.2018.Applications and factors influencing of the persulfate-based advanced oxidation processes for the remediation of groundwater and soil contaminated with organic compounds[J].Journal of Hazardous Materials,359:396-407
Zrinyi N,Pham A L.2017.Oxidation of benzoic acid by heat-activated persulfate:Effect of temperature on transformation pathway and product distribution[J].Water Research,120:43-51