土壤铵氮在热活化过硫酸盐氧化过程中的转化

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Abstract In order to explore the transformation and fate of soil NH₄⁺ in the thermally activated PS oxidation process, this study used soil samples collected from Jiangsu and Hebei provinces with different soil organic matter content and NH₄⁺ concentration to conduct experiments, and systematically investigated effects of persulfate (PS) concentration, the addition of NH₄⁺, and reaction time on the formation of nitro by-products. Results show that soil NH₄⁺ could be transformed to nitrated byproducts, including 3-nitrophenol, 4-nitrophenol, 2-hydroxy-5-nitrobenzoic acid, 4-hydroxy-3-nitrobenzoic acid, 2, 4-dinitrophenol, etc. The formation of nitro by-products increased first and then decreased with reaction time. An increased in PS dose would promote the formation of nitro by-products, and the yields of mono-nitrophenols and hydroxy-mono-nitrobenzoic acids reached the maximum after 12h reaction at 30mmol/kg PS dose. However, nitrated byproducts were degraded at higher PS dose. Note that sulfate radicals (SO₄·^-) played a key role in the nitration process by oxidizing NH₄⁺ to form aminyl radicals (·NH₂), and then underwent a series of free radical chain reactions to form nitrogen dioxide radicals (NO₂·). Besides, phenol moieties in soil organic matter served as the main reactive sites for SO₄·^- attack, leading to the formation of phenoxy radicals, which further combined with NO₂· to form nitro by-products. NOM is everywhere and NH₄⁺ is ubiquitous in the environment. Thus, the formation of nitro by-products will be widespread when PS is applied for contaminated soil and groundwater remediation, which should be taken into consideration when evaluating the feasibility of this technology. This study reveals that the presence of soil NH₄⁺ in activated PS oxidation processes could induce the nitration of NOM and the formation of nitrophenolic by-products.

Key words： ammonium persulfate soil organic matter sulfate radical nitrogen dioxide radical nitrated byproducts

Received: 04 June 2021

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X703.5

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	YANG Pei-zeng
	YUE Hong-shen
	JI Yue-fei
	LU Jun-he

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YANG Pei-zeng,YUE Hong-shen,JI Yue-fei等. Transformation of soil ammonium nitrogen in the process of thermally activated persulfate oxidation[J]. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(1): 267-275.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2022/V42/I1/267

[1]	Tsitonaki A, Petri B, Crimi M, et al. In situ chemical oxidation of contaminated soil and groundwater using persulfate: A review [J]. Critical Reviews in Environmental Science and Technology, 2010, 40(1): 55-91.
[2]	Long A H, Lei Y, Zhang H. In situ chemical oxidation of organic contaminated soil and groundwater using activated persulfate process [J]. Progress in Chemistry, 2014, 26(5): 898-908.
[3]	Zhang B, Zhang Y, Teng Y, et al. Sulfate radical and its application in decontamination technologies [J]. Critical Reviews in Environmental Science and Technology, 2015, 45(16): 1756-1800.
[4]	Matzek L W, Carter K E. Activated persulfate for organic chemical degradation: A review [J]. Chemosphere, 2016, 151: 178-188.
[5]	Zhou Y, Xiang Y, He Y, et al. 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, 2018, 359: 396-407.
[6]	Neta P, Huie R, Ross A. Rate constants for reactions of inorganic radicals in aqueous solution [J]. Journal of Physical and Chemical Reference Data, 1988, 17(3): 1027-1284.
[7]	Liang C, Lee I L, Hsu I Y, et al. Persulfate oxidation of trichloroethylene with and without iron activation in porous media[J]. Chemosphere, 2008, 70(3): 426-435.
[8]	Usman M, Faure P, Ruby C, et al. Application of magnetite-activated persulfate oxidation for the degradation of PAHs in contaminated soils [J]. Chemosphere, 2012, 87(3): 234-240.
[9]	Qian Y, Guo X, Zhang Y, et al. Perfluorooctanoic acid degradation using UV-persulfate process: Modeling of the degradation and chlorate formation [J]. Environmental Science & Technology, 2016, 50 (2): 772-781.
[10]	Bruton T A, Sedlak D L. Treatment of perfluoroalkyl acids by heat-activated persulfate under conditions representative of in situ chemical oxidation [J]. Chemosphere, 2018, 206: 457-464.
[11]	Waldermer R, Tratnyek P, Johnson R, et al. Oxidation of chlorinated ethenes by heat activated persulfate: Kinetics and products [J]. Environmental Science & Technology, 2007, 41(3): 1010-1015.
[12]	刘小宁. 利用热活化过硫酸盐修复氯苯污染地下水的研究[D]. 上海: 华东理工大学, 2013. Liu X N. Remediation of chlorobenzene-contaminated groundwater by thermally activated persulfate [D]. Shanghai: East China University of Science and Technology, 2013.
[13]	Liu Y, Wang S, Wu Y, et al. Degradation of ibuprofen by thermally activated persulfate in soil systems [J]. Chemical Engineering Journal, 2019, 356: 799-810.
[14]	吴承梓, 张巍, 万彦涛, 等. 盐酸羟胺/铁基MOFs/过硫酸盐体系降解磺胺嘧啶[J]. 中国环境科学, 2021, 41(6): 2685-2697. Wu C Z, Zhang W, Wan Y T, et al. Degradation of sulfadiazine by hydroxylamine hydrochloride/Fe-MOFs/persulfate system [J]. China Environmental Science, 2021, 41(6): 2685-2697.
[15]	Lu J, Wu J, Ji Y, et al. Transformation of bromide in thermo activated persulfate oxidation processes [J]. Water Research, 2015, 78: 1-8.
[16]	Fang J, Shang C. Bromate formation from bromide oxidation by the UV/persulfate process [J]. Environmental Science & Technology, 2012, 46(16): 8976-8983.
[17]	Wang Y, Roux J L, Zhang T, et al. Formation of brominated disinfection byproducts from natural organic matter isolates and model compounds in a sulfate radical-based oxidation process [J]. Environmental Science & Technology, 2014, 48(24): 14534-14542.
[18]	Wang L, Kong D, Ji Y, et al. Transformation of iodide and formation of iodinated by-products in heat activated persulfate oxidation process [J]. Chemosphere, 2017, 181: 400-408.
[19]	Ji Y, Wang L, Jiang M, et al. The role of nitrite in sulfate radical-based degradation of phenolic compounds: An unexpected nitration process relevant to groundwater remediation by in-situ chemical oxidation (ISCO) [J]. Water Research, 2017, 123: 249-257.
[20]	Yang P, Ji Y, Lu J, et al. Formation of nitrophenolic byproducts during heat-activated peroxydisulfate oxidation in the presence of natural organic matter and nitrite [J]. Environmental Science & Technology, 2019, 53(8): 4255-4264.
[21]	Yang P, Qian L, Cheng Y, et al. Formation of nitrophenolic byproducts in soils subjected to sulfate radical oxidation [J]. Chemical Engineering Journal, 2021, 403: 126316.
[22]	Barzaghi P, Herrmann H. A mechanistic study of the oxidation of phenol by OH/NO2/NO3in aqueous solution[J]. Physical Chemistry Chemical Physics, 2002, 4(15): 3669-3675.
[23]	Bedini A, Maurino V, Minero C, et al. Theoretical and experimental evidence of the photonitration pathway of phenol and 4-chlorophenol: A mechanistic study of environmental significance [J]. Photochemical & Photobiological Sciences, 2012, 11(2): 418-424.
[24]	Zhang Q, Ren F, Li F, et al. Ammonia nitrogen sources and pollution along soil profiles in an in-situ leaching rare earth ore [J]. Environmental Pollution, 2020, 267: 115449.
[25]	Laszlo B, Alfassi Z B, Neta P, et al. Kinetics and mechanism of the reaction of ·NH2with O2in aqueous solutions [J]. Journal of Physical Chemistry A, 1998, 102: 8498-8504.
[26]	Pagsberg P B. Investigation of the NH2radical produced by pulse radiolysis of ammonia in aqueous solution [R]. Riso National Laboratory Report, Roskilde, Denmark, 1972, 256: 209-221.
[27]	Clarke K, Edge R, Johnson V L, et al. Direct observation of ·NH2 reactions with oxygen, amino acids, and melanins[J]. Journal of Physical Chemistry A, 2008, 112(6): 1234-1237.
[28]	Huang L, Li L, Dong W, et al. Removal of ammonia by OH radical in aqueous phase [J]. Environmental Science & Technology, 2008, 42: 8070-8075.
[29]	Dwibedy P, Kishore K, Dey G R, et al. Nitrite formation in the radiolysis of aerated aqueous solutions of ammonia [J]. Radiation Physics and Chemistry, 1996, 48: 743-747.
[30]	Wang J, Song M, Chen B, et al. Effects of pH and H2O2 on ammonia, nitrite, and nitrate transformations during UV254nm irradiation: Implications to nitrogen removal and analysis [J]. Chemosphere, 2017, 184: 1003-1011.
[31]	Zhang X, Ren P, Li W, et al. Synergistic removal of ammonium by monochloramine photolysis [J]. Water Research, 2019, 152: 226-233.
[32]	Stanbury D M. Reduction potentials involving inorganic free radicals in aqueous solution [J]. Advances in Inorganic Chemistry, 1989, 33: 69-138.
[33]	Wu Z, Chen C, Zhu B Z, et al. Reactive nitrogen species are also involved in the transformation of micropollutants by the UV/ monochloramine Process [J]. Environmental Science & Technology, 2019, 53(19): 11142-11152.
[34]	John M, James R B. Photochemistry of nitrite and nitrate in aqueous solution: A review [J]. Journal of Photochemistry and Photobiology A: Chemistry, 1999, 128: 1-13.
[35]	De Laat J, Boudiaf N, Dossier-Berne F. Effect of dissolved oxygen on the photodecomposition of monochloramine and dichloramine in aqueous solution by UV irradiation at 253.7nm [J]. Water Research, 2010, 44(10): 3261-3269.
[36]	Dey G R. Nitrogen compounds' formation in aqueous solutions under high ionizing radiation: An overview [J]. Radiation Physics and Chemistry, 2011, 80(3): 394-402.
[37]	鲍士旦. 土壤农化分析[M]. 3版. 北京: 中国农业出版社, 2013. Bao S D. Soil agrochemical analysis [M]. Third Edition. Beijing: China Agriculture Press, 2013.
[38]	Liang C, Su H W. Identification of sulfate and hydroxyl radicals in thermally activated persulfate [J]. Industrial & Engineering Chemistry Research, 2009, 48: 5558-5562.
[39]	Neta P, Madhavan V, Zemel H, et al. Rate constants and mechanism of reaction of sulfate radical anion with aromatic compounds [J]. Journal of the American Chemical Society, 1977, 99(1): 163-164.
[40]	Gonzalez M C, Braun A M. Vacuum-UV photolysis of aqueous solutions of nitrate: Effect of organic matter I. Phenol [J]. Journal of Photochemistry and Photobiology A: Chemistry, 1996, 93: 7-19.
[41]	Feng Y, Wu D, Zhou Y, et al. A metal-free method of generating sulfate radicals through direct interaction of hydroxylamine and peroxymonosulfate: Mechanisms, kinetics, and implications [J]. Chemical Engineering Journal, 2017, 330: 906-913.
[42]	Ball, A, Chako J O, Edwards G L. Mechanisms of oxidation of nitrogen nucleophiles by peroxodisulfate ion: Nitrite ion and ammonia [J]. Inorganica Chimica Acta, 1985, 99: 49-58.