PDF
(2190KB)
Abstract
• 90% total COD, 95.3% inert COD and 97.2% UV254 were removed.
• High R2 values (over 95%) for all responses were obtained with CCD.
• Operational cost was calculated to be 0.238 €/g CODremoved for total COD removal.
• Fenton oxidation was highly-efficient method for inert COD removal.
• BOD5/COD ratio of leachate concentrate raised from 0.04 to 0.4.
![]()
The primary aim of this study is inert COD removal from leachate nanofiltration concentrate because of its high concentration of resistant organic pollutants. Within this framework, this study focuses on the treatability of leachate nanofiltration concentrate through Fenton oxidation and optimization of process parameters to reach the maximum pollutant removal by using response surface methodology (RSM). Initial pH, Fe2+ concentration, H2O2/Fe2+ molar ratio and oxidation time are selected as the independent variables, whereas total COD, color, inert COD and UV254 removal are selected as the responses. According to the ANOVA results, the R2 values of all responses are found to be over 95%. Under the optimum conditions determined by the model (pH: 3.99, Fe2+: 150 mmol/L, H2O2/Fe2+: 3.27 and oxidation time: 84.8 min), the maximum COD removal efficiency is determined as 91.4% by the model. The color, inert COD and UV254 removal efficiencies are determined to be 99.9%, 97.2% and 99.5%, respectively, by the model, whereas the total COD, color, inert COD and UV254 removal efficiencies are found respectively to be 90%, 96.5%, 95.3% and 97.2%, experimentally under the optimum operating conditions. The Fenton process improves the biodegradability of the leachate NF concentrate, increasing the BOD5/COD ratio from the value of 0.04 to the value of 0.4. The operational cost of the process is calculated to be 0.238 €/g CODremoved. The results indicate that the Fenton oxidation process is an efficient and economical technology in improvement of the biological degradability of leachate nanofiltration concentrate and in removal of resistant organic pollutants.
Graphical abstract
Keywords
Concentrated leachate
/
Fenton oxidation
/
Central composite design
/
Biodegradability
/
Inert COD
Cite this article
Download citation ▾
Senem Yazici Guvenc, Gamze Varank.
Degradation of refractory organics in concentrated leachate by the Fenton process: Central composite design for process optimization.
Front. Environ. Sci. Eng., 2021, 15(1): 2 DOI:10.1007/s11783-020-1294-1
| [1] |
Abedinzadeh N, Shariat M, Monavari S M, Pendashteh A (2018). Evaluation of color and COD removal by Fenton from biologically (SBR) pre-treated pulp and paper wastewater. Process Safety and Environmental Protection, 116: 82–91
|
| [2] |
Amaral M C S, Moravia W G, Lange L C, Zico M R, Magalhães N C, Ricci B C, Reis B G (2016). Pilot aerobic membrane bioreactor and nanofiltration for municipal landfill leachate treatment. Journal of Environmental Science and Health Part A, 51: 640–649
|
| [3] |
Amr S S A, Aziz H A, Adlan M N, Aziz S Q (2013). Effect of Ozone and Ozone/Fenton in the advanced oxidation process on biodegradable characteristics of semi-aerobic stabilized leachate. Clean- Soil, Air. Water (Basel), 41(2): 148–152
|
| [4] |
APHA (2005). Standard Methods for the Examination of Water and Wastewater,21st ed. Washington, DC: American Public Health Association
|
| [5] |
Bajpai S, Gupta S K, Dey A, Jha M K, Bajpai V, Joshi S, Gupta A (2012). Application of central composite design approach for removal of chromium(VI) from aqueous solution using weakly anionic resin: modelling, optimization, and study of interactive variables. Journal of Hazardous Materials, 227–228: 436–444
|
| [6] |
Biglarijoo N, Mirbagheri S A, Ehteshami M, Ghaznavi S M (2016). Optimization of Fenton process using response surface methodology and analytic hierarchy process for landfill leachate treatment. Process Safety and Environmental Protection, 104: 150–160
|
| [7] |
Borràs N, Oliver R, Arias C, Brillas E (2010). Degradation of atrazine by electrochemical advanced oxidation processes using a boron-doped diamond anode. Journal of Physical Chemistry A, 114(24): 6613–6621
|
| [8] |
Boumechhour F, Rabah K, Lamine C, Said B M (2013). Treatment of landfill leachate using Fenton process and coagulation/flocculation. Water and Environment Journal : the Journal / the Chartered Institution of Water and Environmental Management, 27(1): 114–119
|
| [9] |
Calabrò P S, Sbaffoni S, Orsi S, Gentili E, Meoni C (2010). The landfill reinjection of concentrated leachate: Findings from a monitoring study at an Italian site. Journal of Hazardous Materials, 181(1-3): 962–968
|
| [10] |
Chen W, Zhang A, Gu Z, Li Q (2018). Enhanced degradation of refractory organics in concentrated landfill leachate by Fe0/H2O2 coupled with microwave irradiation. Chemical Engineering Journal, 354: 680–691
|
| [11] |
Cortez S, Teixeira P, Oliveira R, Mota M (2011). Evaluation of Fenton and ozone-based advanced oxidation processes as mature landfill leachate pre-treatments. Journal of Environmental Management, 92: 749–755
|
| [12] |
Cui Y H, Xue W J, Yang S Q, Tu J L, Guo X L, Liu Z Q (2018). Electrochemical/peroxydisulfate/Fe3+ treatment of landfill leachate nanofiltration concentrate after ultrafiltration. Chemical Engineering Journal, 353: 208–217
|
| [13] |
Fernandes A, Labiadh L, Ciríaco L, Pacheco M J, Gadri A, Ammar S, Lopes A (2017). Electro-Fenton oxidation of reverse osmosis concentrate from sanitary landfill leachate: Evaluation of operational parameters. Chemosphere, 184: 1223–1229
|
| [14] |
García-Rodríguez O, Bañuelos J A, El-Ghenymy A, Godínez L A, Brillas E, Rodríguez-Valadez F J (2016). Use of a carbon felt-iron oxide air-diffusion cathode for the mineralization of Malachite Green dye by heterogeneous electro-Fenton and UVA photo electro-Fenton processes. Journal of Electroanalytical Chemistry, 767: 40–48
|
| [15] |
Gulkaya I, Surucu G A, Dilek F B (2006). Importance of H2O2/Fe2+ ratio in Fenton’s treatment of a carpet dyeing wastewater. Journal of Hazardous Materials, 136(3): 763–769
|
| [16] |
He R, Tian B H, Zhang Q Q, Zhang H T (2015). Effect of Fenton oxidation on biodegradability, biotoxicity and dissolved organic matter distribution of concentrated landfill leachate derived from a membrane process. Waste Management (New York, N.Y.), 38: 232–239
|
| [17] |
Hodaifa G, Ochando-Pulido J M, Rodriguez-Vives S, Martinez-Ferez A (2013). Optimization of continuous reactor at pilot scale for olive-oil mill wastewater treatment by Fenton-like process. Chemical Engineering Journal, 220: 117–124
|
| [18] |
Hsueh C L, Huang Y H, Wang C C, Chen C Y (2005). Degradation of azo dyes using low iron concentration of Fenton and Fenton-like system. Chemosphere, 58(10): 1409–1414
|
| [19] |
Hu C J, Huang D L, Zeng G M, Cheng M, Gong X M, Wang R Z, Xue W J, Hu Z X, Liu Y N (2018a). The combination of Fenton process and phanerochaete chrysosporium for the removal of bisphenol A in river sediments: mechanism related to extracellular enzyme, organic acid and iron. Chemical Engineering Journal, 338: 432–439
|
| [20] |
Hu X, Wang X, Ban Y, Ren B (2011). A comparative study of UV-Fenton, UV–H2O2 and Fenton reaction treatment of landfill leachate. Environmental Technology, 32(9): 945–951
|
| [21] |
Hu Y, Lu Y, Liu G, Luo H, Zhang R, Cai X (2018b). Effect of the structure of stacked electro-Fenton reactor on treating nanofiltration concentrate of landfill leachate. Chemosphere, 202: 191–197
|
| [22] |
Iskander S M, Novak J T, He Z (2019). Reduction of reagent requirements and sludge generation in Fenton’s oxidation of landfill leachate by synergistically incorporating forward osmosis and humic acid recovery. Water Research, 151: 310–317
|
| [23] |
Jing X, Cao Y, Zhang X, Wang D, Wu X, Xu H (2011). Biosorption of Cr(VI) from simulated wastewater using a cationic surfactant modified spent mushroom. Desalination, 269(1-3): 120–127
|
| [24] |
Kang K H, Shin H S, Park H (2002). Characterization of humic substances present in landfill leachates with different landfill ages and its implications. Water Research, 36(16): 4023–4032
|
| [25] |
Kjeldsen P, Barlaz M A, Rooker A P, Baun A, Ledin A, Christensen T H (2002). Present and long-term composition of MSW landfill leachate: A review. Critical Reviews in Environmental Science and Technology, 32(4): 297–336
|
| [26] |
Kliś S, Thomas M, Barbusiński K, Gołombek K, Krzemiński Ł, Chyc M (2019). Removal of Azo Dye Acid Red 27 from aqueous solutions using classical and modified Fenton reagent with zero-valent iron. Fibres & Textiles in Eastern Europe, 137: 100–106
|
| [27] |
Li J, Zhao L, Qin L, Tian X, Wang A, Zhou Y, Meng L, Chen Y (2016). Removal of refractory organics in nanofiltration concentrates of municipal solid waste leachate treatment plants by combined Fenton oxidative-coagulation with photo-Fenton processes. Chemosphere, 146: 442–449
|
| [28] |
Li X H, Chen S, Angelidaki I, Zhang Y F (2018). Bio-electro-Fenton processes for wastewater treatment: Advances and prospects. Chemical Engineering Journal, 354: 492–506
|
| [29] |
Long Y, Xu J, Shen D, Du Y, Feng H (2017). Effective removal of contaminants in landfill leachate membrane concentrates by coagulation. Chemosphere, 167: 512–519
|
| [30] |
Mojiri A, Ziyang L, Hui W, Ahmad Z, Tajuddin R M, Abu Amr S S, Kindaichi T, Aziz H A, Farraji H (2017). Concentrated landfill leachate treatment with a combined system including electro-ozonation and composite adsorbent augmented sequencing batch reactor process. Process Safety and Environmental Protection, 111: 253–262
|
| [31] |
Nakhate P H, Patil H G, Marathe K V (2018). Intensification of landfill leachate treatment by advanced Fenton process using classical and statistical approach. Chemical Engineering & Processing: Process Intensification, 133: 148–159
|
| [32] |
Nieto L M, Hodaifa G, Rodríguez S, Giménez J A, Ochando J (2011). Degradation of organic matter in olive-oil mill wastewater through homogeneous Fenton-like reaction. Chemical Engineering Journal, 173(2): 503–510
|
| [33] |
Ölmez T (2009). The optimization of Cr(VI) reduction and removal by electrocoagulation using response surface methodology. Journal of Hazardous Materials, 162(2–3): 1371–1378
|
| [34] |
Oulego P, Collado S, Laca A, Díaz M (2016). Impact of leachate composition on the advanced oxidation treatment. Water Research, 88: 389–402
|
| [35] |
Panda N, Sahoo H, Mohapatra S (2011). Decolourization of methyl orange using Fenton-like mesoporous Fe2O3-SiO2 composite. Journal of Hazardous Materials, 185(1): 359–365
|
| [36] |
Panizza M, Cerisola G (2009). Electro-Fenton degradation of synthetic dyes. Water Research, 43(2): 339–344
|
| [37] |
Peng Y (2017). Perspectives on technology for landfill leachate treatment. Arabian Journal of Chemistry, 10: S2567-S2574
|
| [38] |
Poulopoulos S G, Nikolaki M, Karampetsos D, Philippopoulos C J (2008). Photochemical treatment of 2-chlorophenol aqueous solutions using ultraviolet radiation, hydrogen peroxide and photo-Fenton reaction. Journal of Hazardous Materials, 153(1-2): 582–587
|
| [39] |
Ramaswami S, Behrendt J, Otterpohl R (2018). Comparison of NF-RO and RO-NF for the treatment of mature landfill leachates: A guide for landfill operators. Membranes, 8(2): 17
|
| [40] |
Renou S, Givaudan J G, Poulain S, Dirassouyan F, Moulin P (2008). Landfill leachate treatment: Review and opportunity. Journal of Hazardous Materials, 150(3): 468–493
|
| [41] |
Rivas F J, Beltran F J, Frades J, Buxeda P (2001). Oxidation of p-hydroxybenzoic acid by Fenton’s reagent. Water Research, 35(2): 387–396
|
| [42] |
Sabour M R, Amiri A (2017). Comparative study of ANN and RSM for simultaneous optimization of multiple targets in Fenton treatment of landfill leachate. Waste Management (New York, N.Y.), 65: 54–62
|
| [43] |
Saini R, Kumar P (2016). Optimization of chlorpyrifos degradation by Fenton oxidation using CCD and ANFIS computing technique. Journal of Environmental Chemical Engineering, 4(3): 2952–2963
|
| [44] |
Sevimli M F (2005). Post-treatment of pulp and paper industry wastewater by advanced oxidation processes. Ozone Science and Engineering, 27(1): 37–43
|
| [45] |
Singh S K, Tang W Z, Tachiev G (2013). Fenton treatment of landfill leachate under different COD loading factors. Waste Management, 33: 2116–2122 doi: 10.1016/j.wasman.2013.06.019
|
| [46] |
Smaoui Y, Mseddi S, Ayadi N, Sayadi S, Bouzid J (2019). Evaluation of influence of coagulation/flocculation and Fenton oxidation with iron on landfill leachate treatment. Environment Protection Engineering, 45(1): 139–153
|
| [47] |
Sruthi T, Gandhimathi R, Ramesh S T, Nidheesh P V (2018). Stabilized landfill leachate treatment using heterogeneous Fenton and electro-Fenton processes. Chemosphere, 210: 38–43
|
| [48] |
Subramaniam R, Gang D D, Nie J, Bajpai R, Dufreche R, Baudier J, Sharp R, Zappi M E (2017). Application of response surface methodology for optimization of treatment for an aged landfill leachate using Fenton’s oxidation reagent. Environmental Engineering Science, 34: 731–739
|
| [49] |
Teng C, Zhou K, Zhang Z, Peng C, Chen W (2020). Elucidating the structural variation of membrane concentrated landfill leachate during Fenton oxidation process using spectroscopic analyses. Environmental Pollution, 256: 113467
|
| [50] |
Thomas M, Białecka B, Zdebik D (2017). Removal of organic compounds from wastewater originating from the production of printed circuit boards by UV-Fenton method. Archives of Environmental Protection, 43(4): 39–49
|
| [51] |
Thomas M, Zdebik D (2019). Treatment of real textile wastewater by using potassium Ferrate(VI) and Fe(III)/H2O2: Application of Aliivibrio fischeri and Brachionus plicatilis tests for toxicity assessment. Fibres & Textiles in Eastern Europe, 27: 78–84
|
| [52] |
Thomas M, Zdebik D, Niewiara E (2018). Removing phenols from post-processing wastewater originating from underground coal gasification using coagulation-flocculation and the H2O2/UV process. Polish Journal of Environmental Studies, 27(6): 2757–2763
|
| [53] |
Wang G, Lu G, Zhao J, Yin P, Zhao L (2016a). Evaluation of toxicity and estrogenicity of the landfill-concentrated leachate during advanced oxidation treatment: Chemical analyses and bioanalytical tools. Environmental Science and Pollution Research International, 23: 16015–16024
|
| [54] |
Wang G, Lu G, Yin P, Zhao L, Jimmy Yu Q (2016b). Genotoxicity assessment of membrane concentrates of landfill leachate treated with Fenton reagent and UV-Fenton reagent using human hepatoma cell line. Journal of Hazardous Materials, 307: 154–162
|
| [55] |
Wang H, Wang Y, Li X, Sun Y, Wu H, Chen D (2016c). Removal of humic substances from reverse osmosis (RO) and nanofiltration (NF) concentrated leachate using continuously ozone generation-reaction treatment equipment. Waste Management (New York, N.Y.), 56: 271–279
|
| [56] |
Wang Q, Tian S L, Ning P (2014). Degradation mechanism of methylene blue in a heterogeneous Fenton-like reaction catalyzed by ferrocene. Industrial & Engineering Chemistry Research, 53(2): 643–649
|
| [57] |
Wu Y, Zhou S, Qin F, Peng H, Lai Y, Lin Y (2010). Removal of humic substances from landfill leachate by Fenton oxidation and coagulation. Process Safety and Environmental Protection, 88(4): 276–284
|
| [58] |
Xu J, Long Y, Shen D, Feng H, Chen T (2017). Optimization of Fenton treatment process for degradation of refractory organics in pre-coagulated leachate membrane concentrates. Journal of Hazardous Materials, 323: 674–680
|
| [59] |
Xue W J, Cui Y H, Liu Z Q, Yang S Q, Li J Y, Guo X L (2020). Treatment of landfill leachate nanofiltration concentrate after ultrafiltration by electrochemically assisted heat activation of peroxydisulfate. Separation and Purification Technology, 231: 115928
|
| [60] |
Yılmaz T, Aygun A, Berktay A, Nas B (2010). Removal of COD and colour from young municipal landfill leachate by Fenton process. Environmental Technology, 31: 1635–1640
|
| [61] |
Zhang A, Gu Z, Chen W, Li Q, Jiang G (2018). Removal of refractory organic pollutants in reverse-osmosis concentrated leachate by Microwave–Fenton process. Environmental Science and Pollution Research International, 25(29): 28907–28916
|
| [62] |
Zhang L, Li A M, Lu Y F, Yan L, Zhong S, Deng C L (2009). Characterization and removal of dissolved organic matter (DOM) from landfill leachate rejected by nanofiltration. Waste Management (New York, N.Y.), 29(3): 1035–1040
|
| [63] |
Zhang M, Dong H, Zhao L, Wang D, Meng D (2019). A review on Fenton process for organic wastewater treatment based on optimization perspective. Science of the Total Environment, 670: 110–121
|
| [64] |
Zhang Q Q, Tian B H, Zhang X, Ghulam A, Fang C R, He R (2013). Investigation on characteristics of leachate and concentrated leachate in three landfill leachate treatment plants. Waste Management (New York, N.Y.), 33(11): 2277–2286
|
| [65] |
Zhang X, Fu J, Zhang Y, Lei L (2008). A nitrogen functionalized carbon nanotube cathode for highly efficient electrocatalytic generation of H2O2 in Electro-Fenton system. Separation and Purification Technology, 64(1): 116–123
|
| [66] |
Zhao J, Ouyang F, Yang Y, Tang W (2020). Degradation of recalcitrant organics in nanofiltration concentrate from biologically pretreated landfill leachate by ultraviolet-Fenton method. Separation and Purification Technology, 235: 116076
|
| [67] |
Zhou B, Yu Z, Wei Q, Long H Y, Xie Y, Wang Y (2016). Electrochemical oxidation of biological pretreated and membrane separated landfill leachate concentrates on boron doped diamond anode. Applied Surface Science, 377: 406–415
|
RIGHTS & PERMISSIONS
Higher Education Press