Skip to main content
Log in

Improved oxidation of refractory organics in concentrated leachate by a Fe2+-enhanced O3/H2O2 process

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Concentrated leachate from membrane processes, which contains a mass of refractory organics and salt, has become a new problem for wastewater engineers. In this study, removal of organic contaminants in concentrated landfill leachate was investigated by applying the ferrous ion (Fe2+) catalyzed O3/H2O2 process. The maximum chemical oxygen demand (COD) and absorbance at 254 nm (UV254) removal efficiencies under the optimal conditions (initial pH = 3.0, Fe2+ dosage = 6.500 mM, H2O2 dosage = 18.8 mM and O3 dosage = 52.65 mg min−1) were 48.82% and 63.59%, respectively. These were higher than those achieved using the Fe2+/O3, O3/H2O2, and O3 processes, and biodegradability of the leachate was improved significantly. Moreover, compared with other processes, the Fe2+ had a stronger catalytic effect. Molecular distribution analysis and three-dimensional excitation and emission matrix analysis both indicated that the fulvic acid and humic acid in the concentrated leachate were greatly degraded. Ultraviolet-visible spectra showed that the Fe2+/O3/H2O2 process mainly destroyed unsaturated bonds and decreased the aromatic degree of the leachate. The reaction mechanism of the Fe2+/O3/H2O2 process mainly was attributed to three factors: (1) O3 and H2O2 reacting to produce OH; (2) H2O2 and O3 decomposing into OH through the oxidation of Fe2+ to Fe3+; and (3) coagulation by Fe (OH)3. The OH can rapidly degrade recalcitrant organics, and coagulation also increases the removal of organic matter. Therefore, the Fe2+/O3/H2O2 process was an effective method for treating concentrated landfill leachate.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  • Abu Amr SS, Aziz HA (2012) New treatment of stabilized leachate by ozone/Fenton in the advanced oxidation process. Waste Manag 32:1693–1698

    CAS  Google Scholar 

  • Abu Amr SS, Aziz HA, Adlan MN, Bashir MJK (2013) Pretreatment of stabilized leachate using ozone/persulfate oxidation process. Chem Eng J 221:492–499

    CAS  Google Scholar 

  • Arslan I (2001) Treatability of a simulated disperse dye-bath by ferrous iron coagulation, ozonation, and ferrous iron-catalyzed ozonation. J Hazard Mater 85:229–241

    CAS  Google Scholar 

  • Atmaca E (2009) Treatment of landfill leachate by using electro-Fenton method. J Hazard Mater 163:109–114

    CAS  Google Scholar 

  • Babuponnusami A, Muthukumar K (2014) A review on Fenton and improvements to the Fenton process for wastewater treatment. J Environ Chem Eng 2:557–572

    CAS  Google Scholar 

  • Bello MM, Abdul Raman AA, Asghar A (2019) A review on approaches for addressing the limitations of Fenton oxidation for recalcitrant wastewater treatment. Process Saf Environ Prot 126:119–140

    CAS  Google Scholar 

  • Birchler Deborah R, Milke Mark W, Marks AL, Luthy Richard G (1994) Landfill leachate treatment by evaporation. J Environ Eng 120:1109–1131

    Google Scholar 

  • Birchler DR, Milke MW, Marks AL, Luthy RG (1994) Landfill leachate treatment by evaporation. J Environ Eng 120:1109–1131

    CAS  Google Scholar 

  • Butt TE, Oduyemi KOK (2003) A holistic approach to concentration assessment of hazards in the risk assessment of landfill leachate. Environ Int 28:597–608

    CAS  Google Scholar 

  • Calabrò PS, Sbaffoni S, Orsi S, Gentili E, Meoni C (2010) The landfill reinjection of concentrated leachate: findings from a monitoring study at an Italian site. J Hazard Mater 181:962–968

    Google Scholar 

  • Calabrò PS, Gentili E, Meoni C, Orsi S, Komilis D (2018) Effect of the recirculation of a reverse osmosis concentrate on leachate generation: a case study in an Italian landfill. Waste Manag 76:643–651

    Google Scholar 

  • Cañizares P, Paz R, Sáez C, Rodrigo MA (2009) Costs of the electrochemical oxidation of wastewaters: a comparison with ozonation and Fenton oxidation processes. J Environ Manag 90:410–420

    Google Scholar 

  • Cardoso JC, Bessegato GG, Boldrin Zanoni MV (2016) Efficiency comparison of ozonation, photolysis, photocatalysis and photoelectrocatalysis methods in real textile wastewater decolorization. Water Res 98:39–46

    CAS  Google Scholar 

  • Chamarro E, Marco A, Esplugas S (2001) Use of fenton reagent to improve organic chemical biodegradability. Water Res 35:1047–1051

    CAS  Google Scholar 

  • Chelme-Ayala P, El-Din MG, Smith DW, Adams CD (2011) Oxidation kinetics of two pesticides in natural waters by ozonation and ozone combined with hydrogen peroxide. Water Res 45:2517–2526

    CAS  Google Scholar 

  • Chen W, Westerhoff P, Leenheer JA, Booksh K (2003) Fluorescence excitation− emission matrix regional integration to quantify spectra for dissolved organic matter. Environ Sci Technol 37:5701–5710

    CAS  Google Scholar 

  • 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. Chem Eng J 354:680–691

    CAS  Google Scholar 

  • Chen C, Feng H, Deng Y (2019a) Re-evaluation of sulfate radical based–advanced oxidation processes (SR-AOPs) for treatment of raw municipal landfill leachate. Water Res 153:100–107

    CAS  Google Scholar 

  • Chen W, Gu Z, Wen P, Li Q (2019b) Degradation of refractory organic contaminants in membrane concentrates from landfill leachate by a combined coagulation-ozonation process. Chemosphere 217:411–422

    CAS  Google Scholar 

  • Chen W, Zhang A, Jiang G, Li Q (2019c) Transformation and degradation mechanism of landfill leachates in a combined process of SAARB and ozonation. Waste Manag 85:283–294

    CAS  Google Scholar 

  • Coble PG (1996) Characterization of marine and terrestrial DOM in seawater using excitation-emission matrix spectroscopy. Mar Chem 51:325–346

    CAS  Google Scholar 

  • Cortez S, Teixeira P, Oliveira R, Mota M (2011) Evaluation of Fenton and ozone-based advanced oxidation processes as mature landfill leachate pre-treatments. J Environ Manag 92:749–755

    CAS  Google Scholar 

  • De Laat J, Gallard H, Ancelin S, Legube B (1999) Comparative study of the oxidation of atrazine and acetone by H2O2/UV, Fe (III)/UV, Fe (III)/H2O2/UV and Fe (II) or Fe (III)/H2O2. Chemosphere 39:2693–2706

    Google Scholar 

  • Del Moro G, Mancini A, Mascolo G, Di Iaconi C (2013) Comparison of UV/H2O2 based AOP as an end treatment or integrated with biological degradation for treating landfill leachates. Chem Eng J 218:133–137

    Google Scholar 

  • Di Palma L, Ferrantelli P, Merli C, Petrucci E (2002) Treatment of industrial landfill leachate by means of evaporation and reverse osmosis. Waste Manag 22:951–955

    Google Scholar 

  • Ding J, Wang K, Wang S, Zhao Q, Wei L, Huang H, Yuan Y, Dionysiou DD (2018) Electrochemical treatment of bio-treated landfill leachate: Influence of electrode arrangement, potential, and characteristics. Chem Eng J 344:34–41

    CAS  Google Scholar 

  • Du Y, Zhou M, Lei L (2006) Role of the intermediates in the degradation of phenolic compounds by Fenton-like process. J Hazard Mater 136:859–865

    CAS  Google Scholar 

  • Fares Al M, Mo'ayyad S, Ahmad S, Mohammad A-S (2008) Impact of Fenton and ozone on oxidation of wastewater containing nitroaromatic compounds. J Environ Sci 20:675–682

    Google Scholar 

  • Francois V, Feuillade G, Matejka G, Lagier T, Skhiri N (2007) Leachate recirculation effects on waste degradation: study on columns. Waste Manag 27:1259–1272

    CAS  Google Scholar 

  • Gu Z, Chen W, Li Q, Wang Y, Wu C, Zhang A (2018) Degradation of recalcitrant organics in landfill concentrated leachate by a microwave-activated peroxydisulfate process. RSC Adv 8:32461–32469

    CAS  Google Scholar 

  • 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 Manag 38:232–239

    CAS  Google Scholar 

  • Hermosilla D, Cortijo M, Huang CP (2009) Optimizing the treatment of landfill leachate by conventional Fenton and photo-Fenton processes. Sci Total Environ 407:3473–3481

    CAS  Google Scholar 

  • Jiang F, Qiu B, Sun D (2018) Advanced degradation of refractory pollutants in incineration leachate by UV/peroxymonosulfate. Chem Eng J 349:338–346

    CAS  Google Scholar 

  • Kurniawan TA, Lo W-h, Chan G (2006a) Radicals-catalyzed oxidation reactions for degradation of recalcitrant compounds from landfill leachate. Chem Eng J 125:35–57

    CAS  Google Scholar 

  • Kurniawan TA, Lo W-h, Chan GYS (2006b) Physico-chemical treatments for removal of recalcitrant contaminants from landfill leachate. J Hazard Mater 129:80–100

    CAS  Google Scholar 

  • Kwon BG, Lee DS, Kang N, Yoon J (1999) Characteristics of p-chlorophenol oxidation by Fenton’s reagent. Water Res 33:2110–2118

    Google Scholar 

  • Li M, Zeng Z, Li Y, Arowo M, Chen J, Meng H, Shao L (2015) Treatment of amoxicillin by O3/Fenton process in a rotating packed bed. J Environ Manag 150:404–411

    CAS  Google Scholar 

  • Li C, Jiang F, Sun D, Qiu B (2017) Catalytic ozonation for advanced treatment of incineration leachate using (MnO2-Co3O4)/AC as a catalyst. Chem Eng J 325:624–631

    CAS  Google Scholar 

  • 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

    CAS  Google Scholar 

  • Mansouri L, Sabelfeld M, Geissen S-U, Bousselmi L (2015) Catalysed ozonation for removal of an endocrine-disrupting compound using the O3/Fenton reagents system. Environ Technol 36:1721–1730

    CAS  Google Scholar 

  • Poyatos JM, Muñio M, Almecija M, Torres J, Hontoria E, Osorio F (2010) Advanced oxidation processes for wastewater treatment: state of the art. Water Air Soil Pollut 205:187

    CAS  Google Scholar 

  • Ranjbar Vakilabadi D, Hassani AH, Omrani G, Ramavandi B (2017) Catalytic potential of Cu/Mg/Al-chitosan for ozonation of real landfill leachate. Process Saf Environ Prot 107:227–237

    CAS  Google Scholar 

  • Renou S, Givaudan JG, Poulain S, Dirassouyan F, Moulin P (2008) Landfill leachate treatment: review and opportunity. J Hazard Mater 150:468–493

    CAS  Google Scholar 

  • Rocha EMR, Vilar VJP, Fonseca A, Saraiva I, Boaventura RAR (2011) Landfill leachate treatment by solar-driven AOPs. Sol Energy 85:46–56

    CAS  Google Scholar 

  • Schirman JP, Delavarenne SY (1979) Hydrogen peroxide in organic chemistry. Edition et Documentation Industrielle, Paris

    Google Scholar 

  • Shen Y, Xu Q, Gao D, Shi H (2017) Degradation of an anthraquinone dye by Ozone/Fenton: response surface approach and degradation pathway. Ozone Sci Eng 39:219–232

    CAS  Google Scholar 

  • Sonntag Cv, Gunten Uv (2012) Chemistry of ozone in water and wastewater treatment: from basic principles to applications

  • Sruthi T, Gandhimathi R, Ramesh ST, Nidheesh PV (2018) Stabilized landfill leachate treatment using heterogeneous Fenton and electro-Fenton processes. Chemosphere 210:38–43

    CAS  Google Scholar 

  • Tizaoui C, Bouselmi L, Mansouri L, Ghrabi A (2007) Landfill leachate treatment with ozone and ozone/hydrogen peroxide systems. J Hazard Mater 140:316–324

    CAS  Google Scholar 

  • Vedrenne M, Vasquez-Medrano R, Prato-Garcia D, Frontana-Uribe BA, Ibanez JG (2012) Characterization and detoxification of a mature landfill leachate using a combined coagulation–flocculation/photo Fenton treatment. J Hazard Mater 205-206:208–215

    CAS  Google Scholar 

  • Viollier E, Inglett PW, Hunter K, Roychoudhury AN, Van Cappellen P (2000) The ferrozine method revisited: Fe (II)/Fe (III) determination in natural waters. Appl Geochem 15:785–790

    CAS  Google Scholar 

  • Volk C, Roche P, Joret J-C, Paillard H (1997) Comparison of the effect of ozone, ozone-hydrogen peroxide system and catalytic ozone on the biodegradable organic matter of a fulvic acid solution. Water Res 31:650–656

    CAS  Google Scholar 

  • von Gunten U (2003) Ozonation of drinking water: Part I. Oxidation kinetics and product formation. Water Res 37:1443–1467

    Google Scholar 

  • Wang H, Shen Y, Lou Z, Zhu N, Yuan H, Liu C (2019) Hydroxyl radicals and reactive chlorine species generation via E+-ozonation process and their contribution for concentrated leachate disposal. Chem Eng J 360:721–727

    CAS  Google Scholar 

  • Wiszniowski J, Robert D, Surmacz-Gorska J, Miksch K, Weber JV (2006) Landfill leachate treatment methods: A review. Environ Chem Lett 4:51–61

    CAS  Google Scholar 

  • Wu C-H (2008) Decolorization of C.I. Reactive Red 2 in O3, Fenton-like and O3/Fenton-like hybrid systems. Dyes Pigments 77:24–30

    CAS  Google Scholar 

  • Ye Z, Zhang H, Zhang X, Zhou D (2016) Treatment of landfill leachate using electrochemically assisted UV/chlorine process: effect of operating conditions, molecular weight distribution and fluorescence EEM-PARAFAC analysis. Chem Eng J 286:508–516

    CAS  Google Scholar 

  • Yetilmezsoy K, Sakar S (2008) Improvement of COD and color removal from UASB treated poultry manure wastewater using Fenton’s oxidation. J Hazard Mater 151:547–558

    CAS  Google Scholar 

  • Yoon J, Cho S, Cho Y, Kim S (1998) The characteristics of coagulation of Fenton reaction in the removal of landfill leachate organics. Water Sci Technol 38:209–214

    CAS  Google Scholar 

  • Žgajnar Gotvajn A, Zagorc-Končan J, Cotman M (2011) Fenton's oxidative treatment of municipal landfill leachate as an alternative to biological process. Desalination 275:269–275

    Google Scholar 

  • Zhang H, Choi HJ, Huang C-P (2005) Optimization of Fenton process for the treatment of landfill leachate. J Hazard Mater 125:166–174

    CAS  Google Scholar 

  • 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 Manag 33:2277–2286

    CAS  Google Scholar 

  • Zhang J, Huang G-Q, Liu C, Zhang R-N, Chen X-X, Zhang L (2018) Synergistic effect of microbubbles and activated carbon on the ozonation treatment of synthetic dyeing wastewater. Sep Purif Technol 201:10–18

    CAS  Google Scholar 

  • Zhao Y (2018) Chapter 2 - Physical and Chemical Treatment Processes for Leachate. In: Youcai Z (Ed.) Pollution Control Technology for Leachate from Municipal Solid Waste. Butterworth-Heinemann, pp. 31-183

  • Zheng Z, Zhang H, He P-J, Shao L-M, Chen Y, Pang L (2009) Co-removal of phthalic acid esters with dissolved organic matter from landfill leachate by coagulation and flocculation process. Chemosphere 75:180–186

    CAS  Google Scholar 

  • Zouboulis AI, Chai X-L, Katsoyiannis IA (2004) The application of bioflocculant for the removal of humic acids from stabilized landfill leachates. J Environ Manag 70:35–41

    Google Scholar 

Download references

Funding

The authors gratefully acknowledge the financial support from China’s National Students’ Platform for Innovation and Entrepreneurship Training Program (201810636158).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Aiping Zhang.

Additional information

Responsible editor: Vítor Pais Vilar

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

ESM 1

(DOCX 109 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Huang, Z., Gu, Z., Wang, Y. et al. Improved oxidation of refractory organics in concentrated leachate by a Fe2+-enhanced O3/H2O2 process. Environ Sci Pollut Res 26, 35797–35806 (2019). https://doi.org/10.1007/s11356-019-06592-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-019-06592-y

Keywords

Navigation