氨三乙酸强化零价铁/过一硫酸盐降解橙黄G

马红芳; 杨浩宇; 田委民; 伍凌斌; 陈秀峰; 邹景

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中国环境科学 ›› 2021, Vol. 41 ›› Issue (4) : 1597-1607.

水污染与控制

氨三乙酸强化零价铁/过一硫酸盐降解橙黄G

马红芳^1,2, 杨浩宇¹, 田委民¹, 伍凌斌¹, 陈秀峰¹, 邹景¹

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Degradation of Orange G by Fe⁰/peroxymonosulfate with nitrilotriacetic acid enhancement

MA Hong-fang^1,2, YANG Hao-yu¹, TIAN Wei-min¹, WU Ling-bin¹, CHEN Xiu-feng¹, ZOU Jing¹

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摘要

采用氨三乙酸（NTA）强化和改善零价铁/过一硫酸盐（Fe⁰/PMS）体系降解水中偶氮染料的氧化效能，以橙黄G （OG）为目标污染物，研究了NTA强化Fe⁰/PMS （NTA/Fe⁰/PMS）体系中OG的降解效果和NTA的强化作用机制，并考察了NTA、Fe⁰、PMS等主要反应物浓度和水中常见的共存物质对OG降解效能的影响.结果表明，NTA能够强化Fe⁰/PMS体系降解OG的氧化效能，且初始pH值对其强化作用有显著影响.中性（pH=7）和酸性（pH=3）条件下，NTA/Fe⁰/PMS体系去除OG的表观速率常数分别较Fe⁰/PMS体系提高了31.3倍和5.5倍；增加NTA、Fe⁰和PMS浓度有助于OG的降解，但NTA超过8mmol/L或PMS超过1.0mmol/L时出现抑制现象；水质背景中，Cl^-的存在促进了OG的降解，HCO₃^-、H₂PO₄^-和腐殖酸则表现为不同程度的抑制作用；NTA/Fe⁰/PMS体系中，主导的活性物种为Fe⁰界面产生的SO₄^·-和·OH，界面作用和均相作用对OG的降解分别贡献了约83.2%和16.8%；加入NTA后，体系中生成的Fe³⁺/Fe²⁺能与其迅速形成络合物，既缓解了Fe⁰表面钝化层的形成，促进Fe⁰界面对PMS的直接活化，又提高了溶液中溶解性铁的浓度，促进均相作用对PMS的活化分解，使NTA/Fe⁰/PMS体系降解OG的氧化效能得到强化和改善.

Abstract

Nitrilotriacetic acid (NTA) was applied to enhance and improve the oxidation efficiency of azo dyes in Fe⁰/PMS system. Taking Orange G (OG) as the target pollutant, the degradation efficiency of OG, the strengthening role of NTA, the effects of NTA, Fe⁰, PMS and general coexistence substances in water on the degradation of OG were studied in Fe⁰/PMS system enhanced with NTA(NTA/Fe⁰/PMS).The results demonstrated that the introduction of NTA could enhance the degradation of OG by Fe⁰/PMS system, and the initial pH had a significant effect on the enhancement. Under neutral (pH=7) and acidic (pH=3) conditions, the apparent rate constants of OG removal by NTA/Fe⁰/PMS system were 31.3 times and 5.5 times higher than those of Fe⁰/PMS system, respectively. Increasing the concentration of NTA, Fe⁰ and PMS facilitated the degradation of OG, but negative effects were observed when NTA or PMS concentration were over 8mmol/L and 1.0mmol/L, respectively. In the context of water quality, the presence of Cl^- promoted the degradation of OG, while HCO₃^-, H₂PO₄^- and Humic Acid showed different degrees of inhibition. In NTA/Fe⁰/PMS system, SO₄^·- and·OH produced at Fe⁰ interface was confirmed to be the dominant active species responsible for OG degradation, and heterogeneous and homogeneous activation of PMS contributed about 83.2% and 16.8% to the degradation of OG, respectively. When adding NTA to Fe⁰/PMS system, Fe³⁺/Fe²⁺ generated could be complexed rapidly with NTA, which not only alleviated the formation of passive layer and promoting the direct activation of PMS on Fe⁰ interface, but also increased the concentration of soluble iron in system, promoting the activation of PMS by homogeneous interaction. Thus, the degradation effect of OG in Fe⁰/PMS system was enhanced by NTA.

导出引用

马红芳, 杨浩宇, 田委民, 伍凌斌, 陈秀峰, 邹景. 氨三乙酸强化零价铁/过一硫酸盐降解橙黄G[J]. 中国环境科学. 2021, 41(4): 1597-1607

MA Hong-fang, YANG Hao-yu, TIAN Wei-min, WU Ling-bin, CHEN Xiu-feng, ZOU Jing. Degradation of Orange G by Fe⁰/peroxymonosulfate with nitrilotriacetic acid enhancement[J]. China Environmental Science. 2021, 41(4): 1597-1607

中图分类号： X703.5

参考文献

[1] 毕晨,施周,周石庆,等. EGCG强化Fe²⁺/过硫酸盐体系降解金橙G的研究[J]. 中国环境科学, 2017,37(10):3722-3728. Bi Chen, Shi Zhou, Zhou Shiqing, et al. Degradation of orange G by Fe²⁺/peroxydisulfate system with enhance of EGCG[J]. China Environmental Science, 2017,37(10):3722-3728.
[2] Cai M, Zhu Y, Wei Z, et al. Rapid decolorization of dye Orange G by microwave enhanced Fenton-like reaction with delafossite-type CuFeO₂[J]. Science of the Total Environment, 2017,580:966-973.
[3] Bai C, Xiong X, Gong W, et al. Removal of rhodamine B by ozone-based advanced oxidation process[J]. Desalination. 2011,278(1-3):84-90.
[4] Saleh T A, Gupta V K. Photo-catalyzed degradation of hazardous dye methyl orange by use of a composite catalyst consisting of multi-walled carbon nanotubes and titanium dioxide[J]. Journal of Colloid and Interface Science, 2012,371(1):101-106.
[5] Tan C, Dong Y, Shi L, et al. Degradation of Orange Ⅱ in ferrous activated peroxymonosulfate system:Efficiency, situ EPR spin trapping and degradation pathway study[J]. Journal of the Taiwan Institute of Chemical Engineers, 2018,83:74-81.
[6] Ghanbari F, Moradi M. Application of peroxymonosulfate and its activation methods for degradation of environmental organic pollutants:Review[J]. Chemical Engineering Journal, 2017,310:41-62.
[7] Wang J, Wang S. Activation of persulfate (PS) and peroxymonosulfate (PMS) and application for the degradation of emerging contaminants[J]. Chemical Engineering Journal, 2018,334:1502-1517.
[8] Barzegar G, Jorfi S, Zarezade V, et al. 4-Chlorophenol degradation using ultrasound/peroxymonosulfate/nanoscale zero valent iron:Reusability, identification of degradation intermediates and potential application for real wastewater[J]. Chemosphere, 2018,201:370-379.
[9] Tan C, Dong Y, Fu D, et al. Chloramphenicol removal by zero valent iron activated peroxymonosulfate system:Kinetics and mechanism of radical generation[J]. Chemical Engineering Journal, 2018,334:1006-1015.
[10] Cao J, Lai L, Lai B, et al. Degradation of tetracycline by peroxymonosulfate activated with zero-valent iron:Performance, intermediates, toxicity and mechanism[J]. Chemical Engineering Journal, 2019,364:45-56.
[11] Yao J, Gao M, Guo X, et al. Enhanced degradation performance of bisphenol M using peroxymonosulfate activated by zero-valent iron in aqueous solution:Kinetic study and product identification[J]. Chemosphere, 2019,221:314-323.
[12] Yang Y, Guo H, Zhang Y, et al. Analysis on the removal of ammonia nitrogen using peroxymonosulfate activated by nanoparticulate zero-valent iron[J]. Chemical Papers, 2017,71(8):1497-1505.
[13] Li Z, Luo S, Yang Y, et al. Highly efficient degradation of trichloroethylene in groundwater based on peroxymonosulfate activation by bentonite supported Fe/Ni bimetallic nanoparticle[J]. Chemosphere, 2019,216:499-506.
[14] Sun S, Zeng X, Lemley A T. Kinetics and mechanism of carbamazepine degradation by a modified Fenton-like reaction with ferric-nitrilotriacetate complexes[J]. Journal of Hazardous Materials, 2013,252-253:155-165.
[15] Motekaitis R J, Martell A E. The iron(Ⅲ) and iron(Ⅱ) complexes of nitrilotriacetic acid[J]. Journal of Coordination Chemistry, 1994,31(1):67-78.
[16] Nancharaiah Y V, Schwarzenbeck N, Mohan T V K, et al. Biodegradation of nitrilotriacetic acid (NTA) and ferric-NTA complex by aerobic microbial granules[J]. Water Research, 2006,40(8):1539-1546.
[17] Li J, Chen Z, Shen J, et al. Influence of phosphate, citrate and nitrilotriacetic acid on the removal of aqueous hexavalent chromium by zero-valent iron at circumneutral pH[J]. Journal of the Taiwan Institute of Chemical Engineers, 2017,80:269-275.
[18] Liang C, Huang C, Mohanty N, et al. A rapid spectrophotometric determination of persulfate anion in ISCO[J]. Chemosphere, 2008,73(9):1540-1543.
[19] Harvey A E, Smart J A, Amis E S. Simultaneous Spectrophotometric Determination of Iron(Ⅱ) and Total Iron with 1,10-Phenanthroline[J]. Analytical Chemistry, 1955,27(1):26-29.
[20] Qi C, Liu X, Ma J, et al. Activation of peroxymonosulfate by base:Implications for the degradation of organic pollutants[J]. Chemosphere, 2016,151:280-288.
[21] Kang Y, Yoon H, Lee W, et al. Comparative study of peroxide oxidants activated by nZVI:Removal of 1,4-Dioxane and arsenic(Ⅲ) in contaminated waters[J]. Chemical Engineering Journal, 2018,334:2511-2519.
[22] Wang Z, Qiu W, Pang S, et al. Further understanding the involvement of Fe(IV) in peroxydisulfate and peroxymonosulfate activation by Fe(Ⅱ) for oxidative water treatment[J]. Chemical Engineering Journal, 2019,371:842-847.
[23] Li X, Liu X, Lin C, et al. Catalytic oxidation of contaminants by Fe⁰activated peroxymonosulfate process:Fe(IV) involvement, degradation intermediates and toxicity evaluation[J]. Chemical Engineering Journal, 2020,382:123013.
[24] Wang Z, Jiang J, Pang S, et al. Is Sulfate Radical Really Generated from Peroxydisulfate Activated by Iron(Ⅱ) for Environmental Decontamination?[J]. Environmental Science & Technology, 2018, 52(19):11276-11284.
[25] Wang Z, Qiu W, Pang S, et al. Effect of chelators on the production and nature of the reactive intermediates formed in Fe(Ⅱ) activated peroxydisulfate and hydrogen peroxide processes[J]. Water Research, 2019,164:114957.
[26] Fang G, Wu W, Liu C, et al. Activation of persulfate with vanadium species for PCBs degradation:A mechanistic study[J]. Applied Catalysis B:Environmental, 2017,202:1-11.
[27] Yang S, Xiao T, Zhang J, et al. Activated carbon fiber as heterogeneous catalyst of peroxymonosulfate activation for efficient degradation of Acid Orange 7in aqueous solution[J]. Separation and Purification Technology, 2015,143:19-26.
[28] Pestovsky O, Bakac A. Reactivity of Aqueous Fe(IV) in Hydride and Hydrogen Atom Transfer Reactions[J]. Journal of the American Chemical Society, 2004,126(42):13757-13764.
[29] Lindsey M E, Tarr M A. Inhibition of Hydroxyl Radical Reaction with Aromatics by Dissolved Natural Organic Matter[J]. Environmental Science & Technology, 2000,34(3):444-449.
[30] Ziajka J, Pasiuk-Bronikowska W. Rate constants for atmospheric trace organics scavenging SO₄^- in the Fe-catalysed autoxidation of S(IV)[J]. Atmospheric Environment, 2005,39(8):1431-1438.
[31] Chen J, Qi Y, Pan X, et al. Mechanistic insights into the reactivity of Ferrate(VI) with phenolic compounds and the formation of coupling products[J]. Water Research, 2019,158:338-349.
[32] Sun S, Zeng X, Li C, et al. Enhanced heterogeneous and homogeneous Fenton-like degradation of carbamazepine by nano-Fe₃O₄/H₂O₂ with nitrilotriacetic acid[J]. Chemical Engineering Journal, 2014,244:44-49.
[33] 潘超.氨基三乙酸强化Fe(Ⅲ)/KHSO₅去除4-氯酚的效能研究[D]. 哈尔滨:哈尔滨工业大学, 2013. Pan Chao. Nitrilotriacetate enhanced Fe³⁺/KHSO₅ oxidation of 4-chlorophenol in water[D]. Harbin:Harbin Institute of Technology, 2013.
[34] Jin Y, Wang X, Sun S, et al. Hydroxyl and sulfate radicals formation in UVA/Fe^Ⅲ-NTA/S₂O₈^2- system:Mechanism and effectiveness in carbamazepine degradation at initial neutral pH[J]. Chemical Engineering Journal, 2019,368:541-552.
[35] Liu H, Wang Q, Wang C, et al. Electron efficiency of zero-valent iron for groundwater remediation and wastewater treatment[J]. Chemical Engineering Journal, 2013,215-216:90-95.
[36] Liang C, Wang Z, Mohanty N. Influences of carbonate and chloride ions on persulfate oxidation of trichloroethylene at 20℃[J]. Science of the Total Environment, 2006,370(2/3):271-277.
[37] Wei X, Gao N, Li C, et al. Zero-valent iron (ZVI) activation of persulfate (PS) for oxidation of bentazon in water[J]. Chemical Engineering Journal, 2016,285:660-670.
[38] Buffle J, Greter F L, Haerdi W. Measurement of complexation properties of humic and fulvic acids in natural waters with lead and copper ion-selective electrodes[J]. Analytical chemistry, 1977,49(2):216-222.
[39] Holger V L, Stephanie B, Insa R, et al. Degradation of chlorotriazine pesticides by sulfate radicals and the influence of organic matter[J]. Environmental Science & Technology, 2015,49(3):1673-1680.
[40] 孙绍芳,李佳龙,邱琪,等. Fe(Ⅵ)/Na₂SO₃体系降解阿特拉津效能[J]. 中国环境科学, 2021,41(1):192-198. Sun Shaofang, Li Jialong, Qiu Qi, et al. Degradation efficiency of atrazine by Fe(VI)/Na₂SO₃ system[J]. China Environmental Science, 2021,41(1):192-198.