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Kinetic and mechanistic effects of NO2- on the degradation of 4-chloro-3,5-dimethylphenol in water by ferrate |
LU Ying, YAO Bin-bin, YANG Pei-zeng, JI Yue-fei, CHEN Jing, LU Jun-he |
Department of Environmental Science and Engineering, Nanjing Agricultural University, Nanjing 210095, China |
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Abstract We investigated the impact of NO2- on degradation efficiency, products, and toxicity of 4-chloro-3,5-dimethylphenol (PCMX) during ferrate (Fe(VI)) oxidation. Results demonstrated that Fe(VI) effectively degraded PCMX in water within the pH range of 7~9, achieving a 100% removal in 5minutes with a [Fe(VI)]:[PCMX] ratio of 10:1. The presence of 0.1~10mg/L humic acid (HA) significantly enhanced PCMX degradation. The addition of NO2- inhibited the reaction, and resulted in the formation of various nitrated byproducts. Quenching experiments indicated that high-valent iron species play a key role in this process. Toxicity assessment suggested that these nitrated byproducts and coupling products exhibited prolonged persistence and biotoxicity. For example, OP-6 and OP-7 have half-lives exceeding 180 days, bioaccumulation factors greater than 5000, and chronic toxicity values less than 1mg/L, which may pose certain environmental risks.
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Received: 02 March 2024
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[1] Liao M, Wei S, Zhao J, et al. Risks of benzalkonium chlorides as emerging contaminants in the environment and possible control strategies from the perspective of ecopharmacovigilance [J]. Ecotoxicology and Environmental Safety, 2023,266:115613,1-15. [2] Milanovic M, Duric L, Milosevic N, et al. Comprehensive insight into triclosan-from widespread occurrence to health outcomes [J]. Environmental Science and Pollution Research, 2023,30(10):25119- 25140. [3] Cutts T A, Robertson C, Theriault S S, et al. Efficacy of microbicides for inactivation of Ebola-Makona virus on a non-porous surface: a targeted hygiene intervention for reducing virus spread [J]. Scientific Reports, 2020,10(1):15247,1-9. [4] Guo Y, Gao J, Cui Y, et al. Chloroxylenol at environmental concentrations can promote conjugative transfer of antibiotic resistance genes by multiple mechanisms [J]. Science of The Total Environment, 2022,816:151599,1-11. [5] Au C K, Jason Chan K K, Chan W, et al. Occurrence and stability of PCMX in water environments and its removal by municipal wastewater treatment processes [J]. Journal of Hazardous Materials, 2023,445:130550,1-9. [6] Kasprzyk-Hordern B, Dinsdale R M, Guwy A J. The removal of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters [J]. Water Research, 2009,43(2):363-380. [7] Xu L, Wang J. Degradation of 4-Chloro-3,5-Dimethylphenol by a heterogeneous fenton-like reaction using nanoscale zero-valent iron catalysts [J]. Environmental Engineering Science, 2013,30(6):294- 301. [8] Song S, Liu Z, He Z, et al. Degradation of the biocide 4-chloro-3, 5-dimethylphenol in aqueous medium with ozone in combination with ultraviolet irradiation: operating conditions influence and mechanism [J]. Chemosphere, 2009,77(8):1043-1051. [9] Li W, Guo H, Wang C, et al. ROS reevaluation for degradation of 4-chloro-3,5-dimethylphenol (PCMX) by UV and UV/persulfate processes in the water: Kinetics, mechanism, DFT studies and toxicity evolution [J]. Chemical Engineering Journal, 2020,390,124610,1-11. [10] Sun Y, Zhao J, Zhang B T, et al. Oxidative degradation of chloroxylenol in aqueous solution by thermally activated persulfate: Kinetics, mechanisms and toxicities [J]. Chemical Engineering Journal, 2019,368:553-563. [11] Dar A A, Pan B, Qin J, et al. Sustainable ferrate oxidation: Reaction chemistry, mechanisms and removal of pollutants in wastewater [J]. Environmental Pollution, 2021,290:117957, 1-15. [12] Sharma V K. Ferrate(VI) and ferrate(V) oxidation of organic compounds: Kinetics and mechanism [J]. Coordination Chemistry Reviews, 2013,257(2):495-510. [13] 李宇,程和发.有机污染物的高铁酸盐氧化去除强化技术研究进展[J]. 环境科学研究, 2022,35(6):1323-1333. Li Y, Cheng H F. Research progress on enhanced oxidation technology for the removal of organic pollutants by Ferrate [J]. Research of Environmental Sciences, 2022,35(6):1323-1333. [14] 许正荣,郑龙,安冬.高锰酸盐、高铁酸盐和臭氧预氧化处理饮用水[J]. 水处理技术, 2019,45(6):116-119,130. Xu Z R, Zheng L, An D. Pre-oxidation of drinking water using permanganate, ferrate, and ozone [J]. Water Treatment Technology, 2019,45(6):116-119,130. [15] Nightingale A M, Hassan S U, Warren B M, et al. A droplet microfluidic-based sensor for simultaneous insitu monitoring of nitrate and nitrite in natural waters [J]. Environmental Science & Technology, 2019,53(16):9677-9685. [16] Muhaidat R, Al-Qudah K, Al-Taani A A, et al. Assessment of nitrate and nitrite levels in treated wastewater, soil, and vegetable crops at the upper reach of Zarqa River in Jordan [J]. Environmental Monitoring and Assessment, 2019,191(3):153,1-11. [17] Konneh M, Wandera S M, Murunga S I, et al. Adsorption and desorption of nutrients from abattoir wastewater: modelling and comparison of rice, coconut and coffee husk biochar [J]. Heliyon, 2021,7(11):e08458,1-10. [18] 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. [19] 陈丹莉,栾天罡,罗丽娟.高铁酸盐对生活污水中药品和个人护理品(PPCPs)的降解研究进展[J]. 环境化学, 2022,41(10):3365-3377. Chen D, Luan T G, Luo L J. Research progress on the degradation of pharmaceuticals and personal care products (PPCPs) in domestic sewage by Ferrate [J]. Environmental Chemistry, 2022,41(10):3365- 3377. [20] Huang Z S, Wang L, Liu Y L, et al. Impact of phosphate on ferrate oxidation of organic compounds: an underestimated oxidant [J]. Environmental Science & Technology, 2018,52(23):13897-13907. [21] Sharma V K. Oxidation of inorganic contaminants by ferrates (VI, V, and IV)-kinetics and mechanisms: A review [J]. Journal of Environmental Management, 2011,92(4):1051-1073. [22] Machala L, Prochazka V, Miglierini M, et al. Direct evidence of Fe(V) and Fe(IV) intermediates during reduction of Fe(VI) to Fe(III): a nuclear forward scattering of synchrotron radiation approach [J]. Physical Chemistry Chemical Physics, 2015,17(34):21787-21790. [23] Wang M, Wei J, Tian B, et al. Role of inorganic ions on the removal efficiencies, transformation and mineralization of tert- butylhydroquinone (TBHQ) oxidized by Fe(VI) [J]. Chemical Engineering Journal, 2022,429:123129,1-8. [24] Tian B, Wu N, Pan X, et al. Ferrate(VI) oxidation of bisphenol E-Kinetics, removal performance, and dihydroxylation mechanism [J]. Water Research, 2022,210:118025,1-10. [25] Zheng Q, Wu N, Qu R, et al. Kinetics and reaction pathways for the transformation of 4-tert-butylphenol by ferrate(VI) [J]. Journal of Hazardous Materials, 2021,401:123405,1-11. [26] Wang H, Liu Y, Jiang J Q. Reaction kinetics and oxidation product formation in the degradation of acetaminophen by ferrate(VI) [J]. Chemosphere, 2016,155:583-590. [27] Song Y, Jiang J, Ma J, et al. Enhanced transformation of sulfonamide antibiotics by manganese(IV) oxide in the presence of model humic constituents [J]. Water Research, 2019,153:200-207. [28] Song Y, Jiang J, Ma J, et al. Influence of different nominal molecular weight fractions of humic acids on phenol oxidation by permanganate [J]. Environmental Science & Technology, 2009,43(21):8332-8337. [29] Huang Z S, Wang L, Liu Y L, et al. Ferrate self-decomposition in water is also a self-activation process: Role of Fe(V) species and enhancement with Fe(III) in methyl phenyl sulfoxide oxidation by excess ferrate [J]. Water Research, 2021,197:117094,1-11. [30] 颉亚玮,汪伟,陈吕军,等.Br-对UV/PDS去除对乙酰氨基酚过程的影响及其转化规律[J]. 环境科学学报, 2023,43(9):57-67. Xie Y W, Wang W, Chen L J, et al. The Effect of Br- on the UV/PDS Process for Acetaminophen Removal and Its Transformation Pathways [J]. Journal of Environmental Sciences, 2023,43(9):57-67. [31] Liu T, Chen J, Li N, et al. Unexpected role of nitrite in promoting transformation of sulfonamide antibiotics by peracetic acid: reactive nitrogen species contribution and harmful disinfection byproduct formation potential [J]. Environmental Science & Technology, 2022, 56(2):1300-1309. [32] Gao X, Zhang Q, Yang Z, et al. Formation of nitrophenolic byproducts during UV-activated peroxydisulfate oxidation in the presence of nitrate [J]. ACS ES&T Engineering, 2022,2(2):222-231. [33] Song Y, Jiang J, Ma J, et al. Oxidation of inorganic compounds by aqueous permanganate: Kinetics and initial electron transfer steps [J]. Separation and Purification Technology, 2017,183:350-357. [34] Balakrishnan A, Kanchinadham S B K, Kalyanaraman C. Assessment on biodegradability prediction of tannery wastewater using EPI Suite BIOWIN model [J]. Environmental Monitoring and Assessment, 2020,192(11):1-9. [35] Pan X, Wei J, Zou M, et al. Products distribution and contribution of (de)chlorination, hydroxylation and coupling reactions to 2,4- dichlorophenol removal in seven oxidation systems [J]. Water Research, 2021,194:116916,1-9. |
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