碱热联合活化过硫酸钠对水中苯酚的去除效果与条件优化Optimization of reaction conditions for the removal of phenol in water by using alkaline thermal co-activated sodium persulfate
吴鹍;申子瑞;陈志文;李超鲲;王文东;
摘要(Abstract):
为研究碱热联合活化过硫酸钠(PS)催化氧化降解酚类污染物的去除效果和影响因素,以苯酚为目标污染物,考察PS投加量、NaOH浓度以及反应温度对苯酚降解效果的作用规律。通过使用甲醇、叔丁醇和三氯甲烷作为自由基淬灭剂的淬灭试验来确定碱热联合活化体系中的主导自由基。结果表明,碱热联合活化PS对苯酚废水的降解效果优于单一碱活化或热活化。反应80 min后,碱热联合活化PS对苯酚的去除率可达98.59%,与单一碱活化和热活化相比分别提高了82.15%和47.23%;苯酚的降解速率随PS浓度(10~50 mmol/L)、NaOH浓度(0.1~1.5 mol/L)和反应温度(25~60℃)升高而增加;通过淬灭试验可确定碱热联合活化体系中同时存在硫酸根自由基(·SO-_4)、羟基自由基(·OH)和超氧自由基(·O-_4)、羟基自由基(·OH)和超氧自由基(·O-_2)。碱的加入改变了过硫酸钠降解苯酚的反应途径。碱热联合活化体系中·O-_2)。碱的加入改变了过硫酸钠降解苯酚的反应途径。碱热联合活化体系中·O-_2和酚盐还原PS共同加快了苯酚的降解过程。
关键词(KeyWords): 环境工程学;碱热联合活化;苯酚;过硫酸钠;自由基
基金项目(Foundation): 国家自然科学基金项目(51578440)
作者(Authors): 吴鹍;申子瑞;陈志文;李超鲲;王文东;
DOI: 10.13637/j.issn.1009-6094.2021.0335
参考文献(References):
- [1] TRI N,THANG P Q,TAN L V,et al.Removal of phenolic compounds from wastewaters by using synthesized Fe-nano zeolite[J].Journal of Water Process Engineering,2019,33:101070.
- [2] 周文敏,傅德黔,孙宗光.中国水中优先控制污染物黑名单的确定[J].环境科学研究,1991,4(6):9-12.ZHOU W M,FU D Q,SUN Z G.Determination of black list of China's priority pollutants in water[J].Research of Environmental Sciences,1991,4(6):9-12.
- [3] 章晋门,陈泉源,杨慧敏.过硫酸盐活化方式与氧化降解有机物效能及其在污染场地修复中的应用[J].化工进展,2020,39(1):1-13.ZHANG J M,CHEN Q Y,YANG H M.Influence of persulfate activation on organic pollutant degradation and application in remediation of contaminated land[J].Chemical Industry and Engineering Progress,2020,39(1):1-13.
- [4] 谷得明,郭昌胜,冯启言,等.基于硫酸根自由基的高级氧化技术及其在环境治理中的应用[J].环境化学,2018,37(11):2489-2508.GU D M,GU C S,FENG Q Y,et al.Sulfate radical-based advanced oxidation processes and its application in environmental remediation[J].Environmental Chemistry,2018,37(11):2489-2508.
- [5] 葛勇建,蔡显威,林翰,等.碱活化过一硫酸盐降解水中环丙沙星[J].环境科学,2017,38(12):5116-5123.GE Y J,CAI X W,LIN H,et al.Base activation of peroxymonosulfate for the degradation of ciprofloxacin in water[J].Environmental Science,2017,38(12):5116-5123.
- [6] QI C D,LIU X T,MA J,et al.Activation of peroxymonosulfate by base:implications for the degradation of organic pollutants[J].Chemosphere,2016,151:280-288.
- [7] 栾海彬,杨立翔,鲁帅,等.热活化过硫酸盐对双酚A的降解及其机理[J].环境工程学报,2016,10(5):2459-2464.LUN H B,YANG L X,LU S,et al.Degradation efficiency and mechanism of bisphenol a by thermally activated persulfate[J].Chinese Journal of Environmental Engineering,2016,10(5):2459-2464.
- [8] 魏红,史京转,李佳霖,等.超声、过硫酸钾协同去除水中诺氟沙星的效果[J].环境科学,2015,36(11):4121-4126.WEI H,SHI J Z,LI J L,et al.Norfloxacin solution degradation under ultrasound,potassium persulfate collaborative system[J].Environmental Science,2015,36(11):4121-4126.
- [9] DHAKA S,KUMAR R,KHAN M A,et al.Aqueous phase degradation of methyl paraben using UV-activated persulfate method[J].Chemical Engineering Journal,2017,321:11-19.
- [10] MA J,LIH Y,CHI L P,et al.Changes in activation energy and kinetics of heat-activated persulfate oxidation of phenol in response to changes in pH and temperature[J].Chemosphere,2017,189:86-93.
- [11] SHANGW T,DONG Z J,LI M,et al.Degradation of diatrizoate in water by Fe(II)-activated persulfate oxidation[J].Chemical Engineering Journal,2019,361:1333-1344.
- [12] LOMINCHAR M A,SANTOS A,MIGUEL E D,et al.Remediation of aged diesel contaminated soil by alkaline activated persulfate[J].Science of the Total Environment,2018,622/623:41-48.
- [13] YANG L,CHEN C S,TU Y J,et al.Heterogeneous degradation of organic pollutants by persulfate activated by CuO-Fe3O4:mechanism,stability,and effects of pH and bicarbonate ions[J].Environmental Science & Technology,2015,49(11):6838-6845.
- [14] AHMAD M,TEEL A L,WATTS R J.Mechanism of persulfate activation by phenols[J].Environmental Science & Technology,2013,47(11):5864-5871.
- [15] 肖鹏飞,姜思佳.活化过硫酸盐氧化法修复有机污染土壤的研究进展[J].化工进展,2018,37(12):4862-4873.XIAO P F,JIANG S J.Research progress in remediation of organic contaminated soil by activated persulfate oxidation[J].Chemical Industry and Engineering Progress,2018,37(12):4862-4873.
- [16] HULING S G,KO S,PARK S,et al.Persulfate oxidation of MTBE- and chloroform-spent granular activated carbon[J].Journal of Hazardous Materials,2011,192(3):1484-1490.
- [17] 朱杰,罗启仕,郭琳,等.碱热活化过硫酸盐氧化水中氯苯的试验[J].环境化学,2013,32(12):2256-2262.ZHU J,LUO Q S,GUO L,et al.Remediation of chlorobenzene-contaminated waste water using a combination of thermal-and alkaline-activated persulfate[J].Environmental Chemistry,2013,32(12):2256-2262.
- [18] 吴楠,王三反,李乐卓,等.碱热活化过硫酸盐降解柴油精制废水中的有机硫化合物[J].环境污染与防治,2019,41(4):435-438,444.WU N,WANG S F,LI Y Z,et al.Degradation of organosulfur compound in wastewater of diesel refining by alkali heat activated persulfate[J].Environmental Pollution & Control,2019,41(4):435-438,444.
- [19] 国家环保局编委会.水和废水监测分析方法[M].第四版.北京:中国环境科学出版社,2002:458-462.Compiling Commission of National Environmental Protection Bureau.Methods of water and waste water inspection and analysis[M].4th ed.Beijing:China Environmental Science Press,2002:458-462.
- [20] FURMAN O S,TEEL A L,AHMAD M,et al.Effect of basicity on persulfate reactivity[J].Journal of Environmental Engineering,2011,137(4):241-247.
- [21] 周阳,应路瑶,于欣,等.碱热联合活化过硫酸钠氧化降解2,4-二氯苯酚研究[J].水处理技术,2021,47(3):68-72.ZHOU Y,YING L Y,YU X,et al.Study on oxidative degradation of 2,4-dichlorophenol by alkaline and thermal co-activated sodium persulfate[J].Technology of Water Treatment,2021,47(3):68-72.
- [22] 郑欢.高级氧化技术处理含酚废水的研究[D].大连:大连工业大学,2012.ZHENG H.Study on the treatment for phenol waste water with advanced oxidation technology[D].Dalian:Dalian Polytechnic University,2012.
- [23] GEORGE P A,DIONYSIOS D D.Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science & Technology,2004,38(13):3705-3712.
- [24] NORZAEE S,TAGHAVI M,DJAHED B,et al.Degradation of penicillin G by heat activated persulfate in aqueous solution[J].Journal of Environmental Management,2018,215:316-323.
- [25] FURMAN O S,TEEL A L,WATTS R J.Mechanism of base activation of persulfate[J].Environmental Science & Technology,2010,44(16):6423-6428.
- [26] LIANG C,SU H W.Identification of sulfate and hydroxyl radicals in thermally activated persulfate[J].Industrial & Engineering Chemistry Research,2009,48(11):472-475.
- [27] 徐西蒙,宗绍燕,刘丹.钢渣碱活化过硫酸盐降解双酚A[J].中国环境科学,2019,39(7):2889-2895.XU X M,ZONG S Y,LIU D.Bisphenol A degradation by base-activated persulfate using steel slag[J].China Environmental Science,2019,39(7):2889-2895.
- [28] BUXTON G V,GREENSTOCK C L,HELMAN W P,et al.Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms and hydroxyl radicals (·OH/·O-) in aqueous solution[J].Journal of Physical and Chemical Reference Data,1988,17(2):513-531.
- [29] LOMINCHAR M A,RODRIGUEZ S,LORENZO D,et al.Phenol abatement using persulfate activated by nZVI,H2O2 and NaOH and development of a kinetic model for alkaline activation[J].Environmental Technology,2018,39(1):35-43.
- [30] HUANGZ H,JI Z Y,ZHAO Y Y,et al.Treatment of wastewater containing 2-methoxyphenol by persulfate with thermal and alkali synergistic activation:kinetics and mechanism[J].Chemical Engineering Journal,2020,380:122411.
- [31] 晁雷,邵雪,胡成,等.高盐废水处理工艺技术研究进展[J].安徽农业科学,2011,39(31):19387-19389,19404.CHAO L,SHAO X,HU C,et al.Research progress on the treatment technology of wastewater with high salinity[J].Journal of Anhui Agricultural Sciences,2011,39(31):19387-19389,19404.
- [32] 李海燕.活化过硫酸盐降解典型有机污染物研究[D].北京:中国石油大学,2018.LI H Y.Investigation of typical organics for activate persulfate degradation[D].Beijing:China University of Petroleum,2018.
- [33] JOHNSON R L,TRATNYEK P G,JOHNSON R O.Persulfate persistence under thermal activation conditions[J].Environmental Science & Technology,2008,42(24):9350-9356.
- [34] 鲁松.热活化过硫酸盐体系降解氧氟沙星的研究[D].长春:吉林大学,2020.LU S.Study on degradation of ofloxacin by thermally activated persulfate system[D].Changchun:Jinlin University,2020.