Reactive blue 19 (RB19) is a toxic anionic dye with an anthraquinone moiety, characterized by its intense color and resistance to degradation. In this article, a three-dimensional electrochemical system was constructed, using Ti/RuO2 as anode and steel plate as cathode, combining electrochemical degradation and activated carbon adsorption. RB19 was partially degraded on the surface of the Ti/RuO2 plate eventually. Simultaneously, the granular activated carbon was polarized under the influence of the electric field during the degradation process, the generation of hydroxyl radical in the system and enhancing the mass transfer capacity and current density was catalyzed. Under the optimal conditions, the three-dimensional system filled with granular activated carbon treated RB19 for 1 h with a removal rate far exceeding that of the two-dimensional system, reaching 82.9%, while its synergistic efficiency reached 39%. Furthermore, the removal rate remained 64.9% after 5 cycles. The results suggested that electrochemical oxidation and adsorption can synergistically treat RB19 in the system. Electrochemical tests verified that the mass transfer rate and current density of the three-dimensional system were significantly enhanced compared to the two-dimensional system. Specially, the mass transfer rate (k) of the three-dimensional system was improved by 10.7% compared to the two-dimensional system, reaching 0.031. Finally, hydroxyl radical was detected through electron paramagnetic resonance test, and the possible degradation pathway of dye was inferred by liquid chromatography-mass spectrometry detection of the intermediates. This method provides a more efficient, eco-friendly, and cost-effective approach for treating dye wastewater.
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References
1.
Acuña-BedoyaJ, Comas-CabralesJA, Alvarez-PuglieseCE, et al.Evaluation of electrolytic reactor configuration for the regeneration of granular activated carbon saturated with methylene blue. Journal of Environmental Chemical Engineering, 2020; 8(5):104074; doi: 10.1016/j.jece.2020.104074
2.
AhmadI, BasuD. Electrochemical treatment of reactive orange 16 dye pollutant using microbial fuel cell as renewable power source. Environmental Engineering Science, 2024; 41(1):29–38; doi: 10.1089/ees.2023.0136
3.
AnantharajS, NodaS, DriessM, et al.The Pitfalls of using potentiodynamic polarization curves for tafel analysis in electrocatalytic water splitting. ACS Energy Lett, 2021:1607–1611; doi: 10.1021/acsenergylett.1c00608
4.
AzamK, ShezadN, ShafiqI, et al.A review on activated carbon modifications for the treatment of wastewater containing anionic dyes. Chemosphere, 2022; 306:135566; doi: 10.1016/j.chemosphere.2022.135566
5.
BabakhaniB, IveyDG. Effect of electrodeposition conditions on the electrochemical capacitive behavior of synthesized manganese oxide electrodes. Journal of Power Sources, 2011; 196(24):10762–10774; doi: 10.1016/j.jpowsour.2011.08.102
6.
ChenY, LiN, ZhangY, et al.Novel low-cost Fenton-like layered Fe-titanate catalyst: Preparation, characterization and application for degradation of organic colorants. J Colloid Interface Sci, 2014; 422:9–15; doi: 10.1016/j.jcis.2014.01.013
7.
ChenS, TangL, FengH, et al.Carbon felt cathodes for electro-Fenton process to remove tetracycline via synergistic adsorption and degradation. Sci Total Environ, 2019; 670:921–931; doi: 10.1016/j.scitotenv.2019.03.086
8.
ChethanaM, SorokhaibamLG, BhandariVM, et al.Green approach to dye wastewater treatment using biocoagulants. ACS Sustainable Chem Eng, 2016; 4(5):2495–2507; doi: 10.1021/acssuschemeng.5b01553
9.
ChoS, KimC, HwangI. Electrochemical degradation of ibuprofen using an activated-carbon-based continuous-flow three-dimensional electrode reactor (3DER). Chemosphere, 2020; 259:127382; doi: 10.1016/j.chemosphere.2020.127382
10.
CornejoOM, OrtizM, AguilarZG, et al.Degradation of acid Violet 19 textile dye by electro-peroxone in a laboratory flow plant. Chemosphere, 2021; 271:129804; doi: 10.1016/j.chemosphere.2021.129804
11.
DaudaMY, ErkurtEA. Investigation of reactive Blue 19 biodegradation and byproducts toxicity assessment using crude laccase extract from Trametes versicolor. J Hazard Mater, 2020; 393:121555; doi: 10.1016/j.jhazmat.2019.121555
12.
DongJ, WuY, WangC, et al.Three-dimensional electrodes enhance electricity generation and nitrogen removal of microbial fuel cells. Bioprocess Biosyst Eng, 2020; 43(12):2165–2174; doi: 10.1007/s00449-020-02402-9
13.
ElsayedNH, AlatawiRAS, AlhawitiOHN, et al.Polyaniline grafted melt-spun PET fibers for anionic dye removal. Desalination and Water Treatment, 2020; 195:334–340; doi: 10.5004/dwt.2020.25888
14.
EnacheTA, Oliveira-BrettAM. Phenol and para-substituted phenols electrochemical oxidation pathways. Journal of Electroanalytical Chemistry, 2011; 655(1):9–16; doi: 10.1016/j.jelechem.2011.02.022
15.
EwuzieU, SaliuOD, DultaK, et al.A review on treatment technologies for printing and dyeing wastewater (PDW). Journal of Water Process Engineering, 2022; 50:103273; doi: 10.1016/j.jwpe.2022.103273
16.
GawankarS, MastenSJ. Persulfate/Peroxide oxidation activated by ferrous ions using methylene blue: Development of a screening technique for the production of radicals. Environmental Engineering Science, 2023; 40(11):614–623; doi: 10.1089/ees.2023.0085
17.
GoyalA, SrivastavaVC. Treatment of highly acidic wastewater containing high energetic compounds using dimensionally stable anode. Chemical Engineering Journal, 2017; 325:289–299; doi: 10.1016/j.cej.2017.05.061
18.
GuoX, DuanX, JiJ, et al.Synthesis of nitrogen and sulfur doped graphene on graphite foam for electro-catalytic phenol degradation and water splitting. J Colloid Interface Sci, 2021; 583:139–148; doi: 10.1016/j.jcis.2020.09.053
19.
GuoX, WangJ. Comparison of linearization methods for modeling the Langmuir adsorption isotherm. Journal of Molecular Liquids, 2019; 296:111850; doi: 10.1016/j.molliq.2019.111850
20.
IsahAU, AbdulraheemG, BalaS, et al.Kinetics, equilibrium and thermodynamics studies of C.I. Reactive Blue 19 dye adsorption on coconut shell based activated carbon. International Biodeterioration & Biodegradation, 2015; 102:265–273; doi: 10.1016/j.ibiod.2015.04.006
21.
KantR. Textile dyeing industry an environmental hazard. NS, 2012; 04(01):22–26; doi: 10.4236/ns.2012.41004
22.
LinJ, YeW, XieM, et al.Environmental impacts and remediation of dye-containing wastewater. Nat Rev Earth Environ, 2023; 4(11):785–803; doi: 10.1038/s43017-023-00489-8
23.
LiuX, ChenZ, DuW, et al.Treatment of wastewater containing methyl orange dye by fluidized three dimensional electrochemical oxidation process integrated with chemical oxidation and adsorption. J Environ Manage, 2022; 311:114775; doi: 10.1016/j.jenvman.2022.114775
24.
LiuX, WangJ. Decolorization and degradation of various dyes and dye-containing wastewater treatment by electron beam radiation technology: An overview. Chemosphere, 2024; 351:141255; doi: 10.1016/j.chemosphere.2024.141255
25.
LiuJJ, YangXF, LiF, et al.Area‐Step Cyclic voltammetry for assessing local electrocatalytic activity of gradient materials. ChemElectroChem, 2019; 6(20):5237–5241; doi: 10.1002/celc.201901512
26.
LouT, XuC, GuoQ, et al.Hydroxyl-/Carboxyl-Rich Graphitic Carbon Nitride/Graphene Oxide composites for efficient photodegradation of reactive Red 195 and antibacterial applications. Langmuir, 2023; 39(1):142–154; doi: 10.1021/acs.langmuir.2c02294
27.
MalakootianM, MoridiA. Efficiency of electro-Fenton process in removing Acid Red 18 dye from aqueous solutions. Process Safety and Environmental Protection, 2017; 111:138–147; doi: 10.1016/j.psep.2017.06.008
28.
MaoZ, ZengZ, XueW, et al.Adsorption of reactive brilliant blue dye from aqueous solution using modified walnut shell: Kinetics, equilibrium, and thermodynamics. Environmental Engineering Science, 2021; 38(10):965–973; doi: 10.1089/ees.2020.0364
29.
NoreenN, KazmiM, FerozeN, et al.Treatment of methylene blue in aqueous solution by electrocoagulation/micro-crystalline cellulosic adsorption combined process. Desalination and Water Treatment, 2020; 203:379–387; doi: 10.5004/dwt.2020.26213
30.
Phan QuangHH, NguyenTP, Duc NguyenDD, et al.Advanced electro-Fenton degradation of a mixture of pharmaceutical and steel industrial wastewater by pallet-activated-carbon using three-dimensional electrode reactor. Chemosphere, 2022; 297:134074; doi: 10.1016/j.chemosphere.2022.134074
31.
QinT, YaoB, ZhouY, et al.The three-dimensional electrochemical processes for water and wastewater remediations: Mechanisms, affecting parameters, and applications. Journal of Cleaner Production, 2023; 408:137105; doi: 10.1016/j.jclepro.2023.137105
32.
RaiA, SirotiyaV, MouryaM, et al.Sustainable treatment of dye wastewater by recycling microalgal and diatom biogenic materials: Biorefinery perspectives. Chemosphere, 2022; 305:135371; doi: 10.1016/j.chemosphere.2022.135371
33.
RaifF-E, AkouzA, HasibA, et al.Adsorption of methylene blue onto raw wastes of argan, date, and olive: Study of kinetics and isotherms. Environmental Engineering Science, 2025; 42(4):166–176; doi: 10.1089/ees.2024.0316
34.
ReghiouaA, BarkatD, JawadAH, et al.Synthesis of Schiff’s base magnetic crosslinked chitosan-glyoxal/ZnO/Fe3O4 nanoparticles for enhanced adsorption of organic dye: Modeling and mechanism study. Sustainable Chemistry and Pharmacy, 2021; 20:100379; doi: 10.1016/j.scp.2021.100379
35.
RenW, ZhangQ, ChengC, et al.Electro-induced carbon nanotube discrete electrodes for sustainable persulfate activation. Environ Sci Technol, 2022; 56(19):14019–14029; doi: 10.1021/acs.est.2c03677
36.
Rodríguez-NarváezOM, PicosAR, Bravo-YumiN, et al.Electrochemical oxidation technology to treat textile wastewaters. Current Opinion in Electrochemistry, 2021; 29:100806; doi: 10.1016/j.coelec.2021.100806
37.
SabaB, ChristyAD, JabeenM. Kinetic and enzymatic decolorization of industrial dyes utilizing plant-based biosorbents: A review. Environmental Engineering Science, 2016; 33(9):601–614; doi: 10.1089/ees.2016.0038
38.
SharmaS, AhammedMM. Application of modified water treatment residuals in water and wastewater treatment: A review. Heliyon, 2023; 9(5):e15796; doi: 10.1016/j.heliyon.2023.e15796
39.
ShiH, WangQ, NiJ, et al.Highly efficient removal of amoxicillin from water by three-dimensional electrode system within granular activated carbon as particle electrode. Journal of Water Process Engineering, 2020; 38:101656; doi: 10.1016/j.jwpe.2020.101656
40.
StuparSL, GrgurBN, RadišićMM, et al.Oxidative degradation of Acid Blue 111 by electro-assisted Fenton process. Journal of Water Process Engineering, 2020; 36:101394; doi: 10.1016/j.jwpe.2020.101394
41.
SudarshanS, HarikrishnanS, RathiBhuvaneswariG, et al.Impact of textile dyes on human health and bioremediation of textile industry effluent using microorganisms: Current status and future prospects. J Appl Microbiol, 2023; 134(2); doi: 10.1093/jambio/lxac064
42.
SurendraBS, VeerabhdraswamyM, AnantharajuKS, et al.Green and chemical-engineered CuFe2O4: Characterization, cyclic voltammetry, photocatalytic and photoluminescent investigation for multifunctional applications. J Nanostruct Chem, 2018; 8(1):45–59; doi: 10.1007/s40097-018-0253-x
43.
TehCM, MohamedAR. Roles of titanium dioxide and ion-doped titanium dioxide on photocatalytic degradation of organic pollutants (phenolic compounds and dyes) in aqueous solutions: A review. J Alloys and Compounds, 2011; 509(5):1648–1660; doi: 10.1016/j.jallcom.2010.10.181
44.
TkaczykA, MitrowskaK, PosyniakA. Synthetic organic dyes as contaminants of the aquatic environment and their implications for ecosystems: A review. Sci Total Environ, 2020; 717:137222; doi: 10.1016/j.scitotenv.2020.137222
45.
VuA-T, TuANT, CamVDT. A Novel Ag/ZnO/g-C3N4 (A/ZCN) Nanocomposite for photocatalytic treatment of organic dyes in aqueous solution. Environmental Engineering Science, 2025; 42(5):189–202; doi: 10.1089/ees.2024.0346
WangJ, GuoX. Adsorption kinetics and isotherm models of heavy metals by various adsorbents: An overview. Critical Reviews in Environmental Science and Technology, 2023; 53(21):1837–1865; doi: 10.1080/10643389.2023.2221157
48.
WangS, WangJ. Electron beam technology coupled to fenton oxidation for advanced treatment of dyeing wastewater: From laboratory to full application. ACS EST Water, 2022; 2(5):852–862; doi: 10.1021/acsestwater.2c00040
49.
WangS, WangJ, ChenC, et al.First full-scale application of electron beam technology for treating dyeing wastewater (30,000 m3/d) in China. Radiation Physics and Chemistry, 2022; 196:110136; doi: 10.1016/j.radphyschem.2022.110136
50.
WazirAH, UllahI, YaqoobK. Chemically activated carbon synthesized from rice husk for adsorption of methylene blue in polluted water. Environmental Engineering Science, 2023; 40(8):307–317; doi: 10.1089/ees.2022.0373
51.
XieJ, XieJ, MillerCJ, et al.Enhanced direct electron transfer mediated contaminant degradation by Fe(IV) using a carbon black-supported Fe(III)-TAML suspension electrode system. Environ Sci Technol, 2023; 57(6):2557–2565; doi: 10.1021/acs.est.2c08467
52.
XieJ, ZhangC, WaiteTD. Hydroxyl radicals in anodic oxidation systems: Generation, identification and quantification. Water Res, 2022; 217:118425; doi: 10.1016/j.watres.2022.118425
53.
XingX, TangJ, YaoS, et al.Electrochemical regeneration of granular activated carbon saturated by p-nitrophenol in BDD anode system. Process Safety and Environmental Protection, 2023; 170:207–214; doi: 10.1016/j.psep.2022.11.082
54.
YuH, CheM, ZhaoB, et al.Enhanced electrosorption of rhodamine B over porous copper-nickel foam electrodes modified with graphene oxide/polypyrrole. Synthetic Metals, 2020; 262:116332; doi: 10.1016/j.synthmet.2020.116332
55.
ZhaoZ, LiS, WangT, et al.In-Situ growing tungsten Sulfide/Carbon nanosheets on sodium titanate nanorods to stabilize Surface-Structure for enhanced Sodium-ion storage. J Colloid Interface Sci, 2022; 611:609–616; doi: 10.1016/j.jcis.2021.12.125
56.
ZhaoS, YiH, TangX, et al.Methyl mercaptan removal from gas streams using metal-modified activated carbon. Journal of Cleaner Production, 2015; 87:856–861; doi: 10.1016/j.jclepro.2014.10.001
57.
ZhuX, NiJ, XingX, et al.Synergies between electrochemical oxidation and activated carbon adsorption in three-dimensional boron-doped diamond anode system. Electrochimica Acta, 2011; 56(3):1270–1274; doi: 10.1016/j.electacta.2010.10.073
