Abstract
A two-step electrochemical process including electrooxidation (EO) and electrocoagulation (EC) was proposed for the tertiary treatment of bio-treated landfill leachate (BTLL). The operating conditions of sole EO and EC technology were optimized via batch tests. Batch tests indicate that EO displayed superior removal efficiency towards color (89%) and UV254 (64%) under optimal experimental conditions. EC with the electrode combinations Fe–Fe-Fe–Fe (four plates, anode–cathode-anode–cathode) performed better than the other electrode combinations (Fe-Al–Fe-Al, Al–Fe-Al–Fe, Al-Al-Al-Al) and showed excellent removal efficiency towards COD (60%) and color (85%). In continuous-flow tests of 13 h, compared to sequential EC-EO process, the sequential EO-EC process was more effective than the sequential EC-EO process in reducing organic matters (COD, TOC) and residual chlorine. The sequential EO-EC process could remove 50% COD, 55% TOC, 72% UV254, and 96% color. The average concentration of residual chlorine in the final effluent of EO-EC process (147 mg/L) was significantly lower than that of EC-EO process (463 mg/L). UV–vis and GC–MS analyses indicate that the BTLL mainly contained humic acid and fulvic acid-like substances with unsaturated bonds. Conjugated unsaturated organics could be degraded into organic of small molecular weight after the sequential EO-EC process. EEM spectroscopic analysis revealed that soluble microbial byproducts became the predominant organics in the final effluent. This work verifies the synergism between EO and EC and provides some insights into the removal and degradation performance of organic substances in BTLL during the sequential EO-EC treatment.
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All data generated or analyzed during this study are included in this article and its supplementary material.
Abbreviations
- BDD:
-
Boron-doped diamond
- BTLL:
-
Bio-treated landfill leachate
- CI:
-
Current intensity
- COD:
-
Chemical oxygen demand
- DO:
-
Dissolved oxygen
- EC:
-
Electrocoagulation
- ED:
-
Electrode distance
- EEM:
-
Excitation-emission matrix
- EO:
-
Electrochemical oxidation
- FA:
-
Fulvic acid
- GC-MS:
-
Gas chromatography-mass spectrometry
- HA:
-
Humic acid
- MBRs:
-
Membrane bioreactors
- MP-P:
-
Monopolar parallel
- NF:
-
Nanofiltration
- RO:
-
Reverse osmosis
- TOC:
-
Total organic carbon
References
Borbón B, Oropeza-Guzman MT, Brillas E, Sirés I (2014) Sequential electrochemical treatment of dairy wastewater using aluminum and DSA-type anodes. Environ Sci Pollut Res 21:8573–8584. https://doi.org/10.1007/s11356-014-2787-x
Can OT, Gazigil L, Keyikoglu R (2022) Treatment of intermediate landfill leachate using different anode materials in electrooxidation process. Environ Prog Sustain Energy 41:11. https://doi.org/10.1002/ep.13722
Deng Y, Chen N, Feng C, Chen F, Wang H, Kuang P, Feng Z, Liu T, Gao Y, Hu W (2019) Treatment of organic wastewater containing nitrogen and chlorine by combinatorial electrochemical system: taking biologically treated landfill leachate treatment as an example. Chem Eng J 364:349–360. https://doi.org/10.1016/j.cej.2019.01.176
Devlin TR, di Biase A, Wei V, Elektorowicz M, Oleszkiewicz JA (2017) Removal of soluble phosphorus from surface water using iron (Fe-Fe) and aluminum (Al-Al) electrodes. Environ Sci Technol 51:13825–13833. https://doi.org/10.1021/acs.est.7b02353
Dia O, Drogui P, Buelna G, Dubé R, Ihsen BS (2017) Electrocoagulation of bio-filtrated landfill leachate: fractionation of organic matter and influence of anode materials. Chemosphere 168:1136–1141. https://doi.org/10.1016/j.chemosphere.2016.10.092
Dobrosz-Gómez I, Gómez-García M-Á (2021) Integration of environmental and economic performance of electro-coagulation-anodic oxidation sequential process for the treatment of soluble coffee industrial effluent. Sci Total Environ 764:142818. https://doi.org/10.1016/j.scitotenv.2020.142818
Fernandes A, Pacheco MJ, Ciriaco L, Lopes A (2015) Review on the electrochemical processes for the treatment of sanitary landfill leachates: present and future. Appl Catal B-Environ 176:183–200. https://doi.org/10.1016/j.apcatb.2015.03.052
Galvão N, de Souza JB, Vidal CMdS (2020) Landfill leachate treatment by electrocoagulation: effects of current density and electrolysis time. J Environ Chem Eng 8:104368. https://doi.org/10.1016/j.jece.2020.104368
Gálvez A, Giusti L, Zamorano M, Ramos-Ridao AF (2009) Stability and efficiency of biofilms for landfill leachate treatment. Bioresour Technol 100:4895–4898. https://doi.org/10.1016/j.biortech.2009.05.014
Ghosh D, Medhi CR, Purkait MK (2008) Treatment of fluoride containing drinking water by electrocoagulation using monopolar and bipolar electrode connections. Chemosphere 73:1393–1400. https://doi.org/10.1016/j.chemosphere.2008.08.041
Heffron J, Ryan DR, Mayer BK (2019) Sequential electrocoagulation-electrooxidation for virus mitigation in drinking water. Water Res 160:435–444. https://doi.org/10.1016/j.watres.2019.05.078
Ibarra-Taquez HN, GilPavas E, Blatchley ER, Gómez-García M-Á, Dobrosz-Gómez I (2017) Integrated electrocoagulation-electrooxidation process for the treatment of soluble coffee effluent: optimization of COD degradation and operation time analysis. J Environ Chem Eng 200:530–538. https://doi.org/10.1016/j.jenvman.2017.05.095
Jiang F, Qiu B (2019) Degradation of refractory organics from biologically treated incineration leachate by VUV/O. Chem Eng J 370:346–353. https://doi.org/10.1016/j.cej.2019.03.206
Kaur R, Kushwaha JP, Singh N (2018) Electro-oxidation of Ofloxacin antibiotic by dimensionally stable Ti/RuO2 anode: evaluation and mechanistic approach. Chemosphere 193:685–694. https://doi.org/10.1016/j.chemosphere.2017.11.065
Keyikoglu R, Karatas O, Rezania H, Kobya M, Vatanpour V, Khataee A (2021) A review on treatment of membrane concentrates generated from landfill leachate treatment processes. Sep Purif Technol 259:25. https://doi.org/10.1016/j.seppur.2020.118182
Lin H, Peng H, Feng X, Li X, Zhao J, Yang K, Liao J, Cheng D, Liu X, Lv S, Xu J, Huang Q (2021) Energy-efficient for advanced oxidation of bio-treated landfill leachate effluent by reactive electrochemical membranes (REMs): laboratory and pilot scale studies. Water Res 190:116790. https://doi.org/10.1016/j.watres.2020.116790
Lin, JY, Raharjo, A, Hsu, LH, 2019. Electrocoagulation of tetrafluoroborate (BF4-) and the derived boron and fluorine using aluminum electrodes. Water Res 155:362–371. https://doi.org/10.1016/j.watres.2019.02.037
Liu YJ, Hu CY, Lo SL (2019) Direct and indirect electrochemical oxidation of amine-containing pharmaceuticals using graphite electrodes. J Hazard Mater 366:592–605. https://doi.org/10.1016/j.jhazmat.2018.12.037
Mandal P, Dubey BK, Gupta AK (2017) Review on landfill leachate treatment by electrochemical oxidation: drawbacks, challenges and future scope. Waste Manage 69:250–273. https://doi.org/10.1016/j.wasman.2017.08.034
Milad, Mousazadeh Zohreh, Naghdali Zakaria, Al-Qodah S.M., Alizadeh Elnaz, Karamati Niaragh Sima, Malekmohammadi P.V., Nidheesh Edward P.L., Roberts Mika, Sillanpää Mohammad, Mahdi Emamjomeh (2021) A systematic diagnosis of state of the art in the use of electrocoagulation as a sustainable technology for pollutant treatment: An updated review. Sustain Energy Technol Assess 47101353-S2213138821003635 101353. https://doi.org/10.1016/j.seta.2021.101353
Mousazadeh M, Naghdali Z, Al-Qodah Z, Alizadeh SM, Niaragh EK, Malekmohammadi S, Nidheesh PV, Roberts E P L, Sillanpaa M, Emamjomeh MM (2021) A systematic diagnosis of state of the art in the use of electrocoagulation as a sustainable technology for pollutant treatment: An updated review. Sustain Energy Technol Assess 47, 24. https://doi.org/10.1016/j.cej.2021.132281
Oumar D, Patrick D, Gerardo B, Rino D, Ihsen BS (2016) Coupling biofiltration process and electrocoagulation using magnesium-based anode for the treatment of landfill leachate. J Environ Manage 181:477–483. https://doi.org/10.1016/j.jenvman.2016.06.067
Philibert M, Luo S, Moussanas L, Yuan Q, Filloux E, Zraick F, Murphy KR (2022) Drinking water aromaticity and treatability is predicted by dissolved organic matter fluorescence. Water Res 220:118592. https://doi.org/10.1016/j.watres.2022.118592
Pikaar I, Flugen M, Lin HW, Salehin S, Li JL, Donose BC, Dennis PG, Bethke L, Johnson I, Rabaey K, Yuan ZG (2019) Full-scale investigation of in-situ iron and alkalinity generation for efficient sulfide control. Water Res 167:8. https://doi.org/10.1016/j.watres.2019.115032
Ryan DR, Maher EK, Heffron J, Mayer BK, McNamara PJ (2021) Electrocoagulation-electrooxidation for mitigating trace organic compounds in model drinking water sources. Chemosphere 273:129377. https://doi.org/10.1016/j.chemosphere.2020.129377
SEPA (2002) Water and Wastewater Monitoring Analysis Method (Fourth ed.), China Environ. Sci. Press Beijing
Sui Q, Zhao WT, Cao XQ, Lu SG, Qiu ZF, Gu XG, Yu G (2017) Pharmaceuticals and personal care products in the leachates from a typical landfill reservoir of municipal solid waste in Shanghai, China: occurrence and removal by a full-scale membrane bioreactor. J Hazard Mater 323:99–108. https://doi.org/10.1016/j.jhazmat.2016.03.047
Shi JY, Sun DZ, Dang Y (2022) Characterizing the degradation of refractory organics from incineration leachate membrane concentrate by VUV/O3. Chem Eng J 428, 10. https://doi.org/10.1016/j.cej.2021.132281
Tejera J, Hermosilla D, Miranda R, Gasco A, Alonso V, Negro C, Blanco A (2020) Assessing an integral treatment for landfill leachate reverse osmosis concentrate. Catalysts 10:17. https://doi.org/10.3390/catal10121389
Tejera J, Hermosilla D, Gascó A, Miranda R, Alonso V, Negro C, Blanco Á (2021) Treatment of mature landfill leachate by electrocoagulation followed by Fenton or UVA-LED photo-Fenton processes. J Taiwan Inst Chem Eng 119:33–44. https://doi.org/10.1016/j.jtice.2021.02.018
Tejera J, Gasco A, Hermosilla D, Alonso-Gomez V, Negro C, Blanco A (2021b) UVA-LED technology’s treatment efficiency and cost in a competitive trial applied to the photo-Fenton treatment of landfill leachate. Processes 9:11. https://doi.org/10.3390/pr9061026
Teng CY, Zhou KG, Peng CH, Chen W (2021) Characterization and treatment of landfill leachate: a review. Water Res 203:13. https://doi.org/10.1016/j.watres.2021.117525
Ulu F, Barisci S, Kobya M, Sarkka H, Sillanpaa M (2014) Removal of humic substances by electrocoagulation (EC) process and characterization of floc size growth mechanism under optimum conditions. Sep Purif Technol 133:246–253. https://doi.org/10.1016/j.seppur.2014.07.003
Ulu F, Gengec E, Kobya M (2019) Removal of natural organic matter from Lake Terkos by EC process: studying on removal mechanism by floc size and zeta potential measurement and characterization by HPSEC method. J Water Process Eng 31:9. https://doi.org/10.1016/j.jwpe.2019.100831
Wang YN, Wang HW, Wu YJ, Sun YJ, Gong ZG, Liu KQ, Tsang YF, Zhan ML (2020) Effective removal of contaminants from biotreated leachate by a combined Fe(III)/O3 process: efficiency and mechanisms. J Cleaner Prod 276:9. https://doi.org/10.1016/j.jclepro.2020.123379
Yang X, De Buyck P-J, Zhang R, Manhaeghe D, Wang H, Chen L, Zhao Y, Demeestere K, Van Hulle SWH (2022) Enhanced removal of refractory humic- and fulvic-like organics from biotreated landfill leachate by ozonation in packed bubble columns. Sci Total Environ 807:150762. https://doi.org/10.1016/j.scitotenv.2021.150762
Zhou B, Yu ZM, Wei QP, Long HY, Xie YN, Wang YJ (2016) Electrochemical oxidation of biological pretreated and membrane separated landfill leachate concentrates on boron doped diamond. Appl Surf Sci 377:406–415. https://doi.org/10.1016/j.apsusc.2016.03.045
Zhu MJ, Yao J, Wang WB, Yin XQ, Chen W, Wu XY (2016) Using response surface methodology to evaluate electrocoagulation in the pretreatment of produced water from polymer-flooding well of Dagang Oilfield with bipolar aluminum electrodes. Desalin Water Treat 57:15314–15325. https://doi.org/10.1080/19443994.2015.1072058
Acknowledgements
Thanks are also expressed to Ph.D. Qigui Niu from the School of Environmental Science and Engineering, Shandong University, for his help in terms of the EEM spectroscopic analyses.
Funding
This study was supported by the Natural Science Foundation of Shandong Province (No. ZR2019MEE046, No. ZR2020QE227) and the Top Discipline in Materials Science of Shandong Province.
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Jianbo Lu: conceptualization, reviewing, and funding acquisition.
Lei Wang: investigation and writing—original draft preparation.
Guifang Si: investigation.
Bin Lu: software and methodology.
Xintong Zhang: reviewing and editing and supervision.
Jie Li: software and data curation.
Wei Zhang: validation.
Zhenhua Wang: investigation and visualization.
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Highlights
• A two-step electrochemical process including EO and EC was proposed for BTLL treatment.
• Sequential EO-EC process was found to outperform EC-EO process via continuous-flow tests.
• Residual chlorine of EO-EC effluent was significantly reduced.
• Conjugated unsaturated organics was degraded into small molecular organics by EO-EC process.
• Soluble microbial byproducts were the predominant organics in the effluent of EO-EC process.
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Lu, J., Wang, L., Si, G. et al. Tertiary treatment of bio-treated landfill leachate by a two-step electrochemical process including electrooxidation and electrocoagulation: a bench-scale trial. Environ Sci Pollut Res 30, 32600–32613 (2023). https://doi.org/10.1007/s11356-022-24028-y
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DOI: https://doi.org/10.1007/s11356-022-24028-y