二价铁活化分子氧体系中溶解氧对活性自由基产生及污染物降解的影响

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Abstract The Fe²⁺/O₂/sodium tripolyphosphate (STPP) advanced oxidation system was constructed to investigate the ability of active radical generation and pollutant degradation under the conditions of continuous aeration and limited dissolved oxygen by aeration and fixed initial DO experiments, respectively. The results showed that under full aeration at a flow rate of 150mL/min, when the concentration of Fe²⁺-STPP increased from 3mmol/L to 20mmol/L, the production of hydroxyl radicals under neutral conditions increased from 0.185mmol/L to 0.256mmol/L, and the removal rate of phenol increased from 81.4% to 91.5%. When the initial DO concentration was fixed in the confined environment and the Fe²⁺-STPP concentration was sufficient, the conversion of O₂ to HO• was about 10.60%~18.05%, and the conversion rate increased with the increase of DO concentration. The amounts of the cumulative HO• produced and the consumed reducing agent Fe²⁺ were quantified, and the response relationship between the amount of pollutants degraded and the initial DO concentration was clarified, and their linear correlation equation was also established (R²>0.99).

Key words： molecular oxygen activation sodium tripolyphosphate (STPP) reactive free radicals dissolved oxygen concentration response relationship ferrous iron contaminant degradation

Received: 08 May 2023

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X703

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	Articles by authors
	WANG Ying-qi
	ZHANG Cheng-wu
	WANG De-yu
	FU Yu-feng
	ZHANG Hui
	QIN Chuan-yu

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WANG Ying-qi,ZHANG Cheng-wu,WANG De-yu等. Effect of dissolved oxygen on reactive free radicals production and pollutant degradation in ferrous ion activated molecular oxygen systems[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(1): 132-139.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I1/132

[1]	赵江涛,周金龙,高业新,等.新疆焉耆盆地平原区地下水有机污染评价及污染成因[J].中国环境科学, 2016,36(1):117-124.Zhao J T, Zhou J L, Gao Y X, et al.Assessment of organic pollution and study on pollution cause of groundwater in the plain area of Yanqi Basin,Xinjiang [J].China Environmental Science, 2016,36(1):117-124.
[2]	杨明星,杨悦锁,杜新强,等.石油污染地下水有机污染组分特征及其环境指示效应[J].中国环境科学, 2013,33(6):1025-1032.Yang M X, Yang Y S, Du X Q, et al.Organic fractions and their environmental implications of petroleum contaminated groundwater [J].China Environmental Science, 2013,33(6):1025-1032.
[3]	乔斐,王锦国,郑诗钰,等.重点区域建设用地污染地块特征分析[J].中国环境科学, 2022,42(11):5265-5275.Qiao F, Wang J G, Zheng S Y, et al.Characterization of contaminated construction sites in key regions [J].China Environmental Science, 2022,42(11):5265-5275.
[4]	施帅帅,王欲晓,庄严,等.Fenton试剂处理工业废水研究进展[J].广州化工, 2017,45(10):20-23,53.Shi S S, Wang Y X, Zhuang Y, et al.Research progress on industrial wastewater by fenton reagent [J].Guangzhou Chemical Industry, 2017, 45(10):20-23,53.
[5]	杨春维.Fenton与电Fenton技术处理有机废水的应用研究[D].大连:大连理工大学, 2012.Yang C W.Fenton and electro-fenton technology for treatment of heterocyclic organic wastewater with modified catalyst [D].Dalian:Dalian University of Technology, 2012.
[6]	王丽.亚铁四聚磷酸活化分子氧高级氧化系统构建及其降解有机污染物性能研究[D].武汉:华中师范大学, 2015.Wang L.Design of advanced oxidation systems with molecular oxygen activation by Fe(Ⅱ)-TPP complex and their performance on organic pollutants degradation [D].Wuhan:Central China Normal University, 2015.
[7]	Watts R J, Finn D D, Cutler L M, et al.Enhanced stability of hydrogen peroxide in the presence of subsurface solids [J].Journal of Contaminant Hydrology, 2007,91(3/4):312-326.
[8]	Xu X, Thomson N R.Hydrogen peroxide persistence in the presence of aquifer materials [J].Soil and Sediment Contamination, 2010,19(5):602-616.
[9]	Minaev B F.Intensities of spin-forbidden transitions in molecular oxygen and selective heavy-atom effects [J].International Journal of Quantum Chemistry, 1980,17(2):367-374.
[10]	Suzuki M, Ishikawa T, Harada A, et al.Chemical mechanism of dioxygen activation by manganese(III) Schiff base compound in the presence of aliphatic aldehydes [J].Polyhedron, 1997,16(15):2553-2561.
[11]	Keenan C R, Sedlak D L.Ligand-enhanced reactive oxidant generation by nanoparticulate zero-valent iron and oxygen [J].Environmental Science & Technology, 2008,42(18):6936-6941.
[12]	Xie W, Zhang P, Liao W, et al.Ligand-enhanced electron utilization for trichloroethylene degradation by·OH during sediment oxygenation [J].Environmental Science & Technology, 2021,55(10):7044-7051.
[13]	Yu C, Zhang Y, Lu Y, et al.Mechanistic insight into humic acid-enhanced hydroxyl radical production from Fe(II)-bearing clay mineral oxygenation [J].Environmental Science & Technology, 2021, 55:13366−13375.
[14]	童曼.地下环境Fe(Ⅱ)活化O2产生活性氧化物种与除砷机制[D].北京:中国地质大学, 2015.Tong M.Activation of O2 by Fe(Ⅱ) in subsurface environments for reactive oxygen species production and arsenic removal [D].Beijing:China University of Geosciences, 2015.
[15]	Pang S Y, Jiang J, Ma J.Oxidation of sulfoxides and arsenic(III) in corrosion of nanoscale zero valent iron by oxygen:evidence against ferryl Ions (Fe(IV)) as active intermediates in fenton reaction [J].Environmental Science & Technology, 2011,45(1):307-312.
[16]	Keenan C R, Sedlak D L.Factors affecting the yield of oxidants from the reaction of nanoparticulate zero-valent iron and oxygen [J].Environmental Science & Technology, 2008,42(4):1262-1267.
[17]	Kantar C, Oral O, Urken O, et al.Role of complexing agents on oxidative degradation of chlorophenolic compounds by pyrite-Fenton process:Batch and column experiments [J].Journal of Hazardous Materials, 2019,373:160-167.
[18]	Zeng Q, Dong H, Wang X.Effect of ligands on the production of oxidants from oxygenation of reduced Fe-bearing clay mineral nontronite [J].Geochimica et Cosmochimica Acta, 2019,251:136-156.
[19]	Kim M S, Kim H H, Lee K M, et al.Oxidation of microcystin-LR by ferrous-tetrapolyphosphate in the presence of oxygen and hydrogen peroxide [J].Water Research, 2017,114:277-285.
[20]	Zhang C, Kong C, Tratnyek P G, et al.Generation of reactive oxygen species and degradation of pollutants in the Fe2+/O2/tripolyphosphate system:regulated by the concentration ratio of Fe2+ and tripolyphosphate [J].Environmental Science & Technology, 2022, 56(7):4367-4376.
[21]	张成武,李天一,廉静茹,等.Fe(Ⅱ)活化O2高级氧化降解罗丹明B染料[J].中国环境科学, 2018,38(2):560-565.Zhang C W, Li T Y, Lian J R, et al.Study on degradation of rhodamine B by advanced oxidation based on O2 activation by Fe(Ⅱ) [J].China Environmental Science, 2018,38(2):560-565.
[22]	Mopper K, Zhou X.Hydroxyl radical photoproduction in the sea and its potential impact on marine processes [J].Science, 1990,250(4981):661-664.
[23]	Lei Y, Yu Y, Lei X, et al.Assessing the use of probes and quenchers for understanding the reactive species in advanced oxidation processes [J].Environmental Science & Technology, 2023,57(13):5433-5444.
[24]	Tamura H, Goto K, Yotsuyanagi T, et al.Spectrophotometric determination of iron(II) with 1,10-phenanthroline in the presence of large amounts of iron(III) [J].Talanta, 1974,21(4):314-318.
[25]	Zong Y, Mao Y, Xu L, et al.Non-selective degradation of organic pollutants via dioxygen activation induced by Fe(II)-tetrapolyphosphate complexes:Identification of reactive oxidant and kinetic modeling [J].Chemical Engineering Journal, 2020,398:25603.
[26]	Zhang C, Li T, Zhang J, et al.Degradation of p-nitrophenol using a ferrous-tripolyphosphate complex in the presence of oxygen:The key role of superoxide radicals [J].Applied Catalysis B:Environmental, 2019,259:118030.
[27]	张成武.基于Fe(Ⅱ)-STPP配合物活化分子氧的高级氧化体系降解对硝基酚的效果及机理[D].长春:吉林大学, 2019.Zhang C W.Reserch on the effect and mechanism of p-nitrophenol degradation by advanced oxidation technology based on activation of molecular oxygen by Fe(ll)-STPP complex [D].Changchun:Jilin University, 2019.
[28]	苗富铭,任高妙,武文莉,等.超重力强化O3/Fe(Ⅱ)氧化降解DNT实际废水[J].含能材料, 2022,30(10):995-1003.Miao F M, Ren G M, Wu W L, et al.Degradation of actual wastewater containing dinitrtoluene with O3/Fe(Ⅱ) oxidation process enhanced by high gravity technology [J].Chinese Journal of Energetic Materials, 2022,30(10):995-1003.
[29]	Yu X Y, Barker J R.Hydrogen peroxide photolysis in acidic aqueous solutions containing chloride Ions.II.Quantum yield of HO• (Aq) radicals [J].The Journal of Physical Chemistry A, 2003,107(9):1325-1332.
[30]	罗翔.有机污染物与羟基自由基和单线态氧水相反应速率常数的QSAR模型[D].大连:大连理工大学, 2021.Luo X.QSAR models for aqueous reaction rate constants of organic pollutants with hydroxyl radical and singlet oxygen [D].Dalian:Dalian University of Technology, 2021.
[31]	姜南.基于自由基处理难降解有机废水的研究[D].大连:大连工业大学, 2015.Jiang N.Study on the treatment for non-biodegradable organic waste water with free radicals [D].Dalian:Dalian Polytechnic University, 2015.
[32]	Huie R E, Clifton C L.Temperature dependence of the rate constants for reactions of the sulfate radical, SO4-, with anions [J].Journal of Physical Chemistry, 1990,94(23):8561-8567.
[33]	马丽娟,令狐珊珊,潘涛,等.铁改性膨润土活化过氧化尿素降解三氯乙烯[J].中国环境科学, 2023,43(5):2434-2439.Ma L J, Linghu S S, Pan T, et al.Iron-modified bentonite activated urea peroxide degrades trichloroethylene [J].China Environmental Science, 2023,43(5):2434-2439.