Skip to main content
SpringerLink
Log in

Investigating the activation of hydrochar from sewage sludge for the removal of terbuthylazine from aqueous solutions

  • ORIGINAL ARTICLE
  • Published:
Journal of Material Cycles and Waste Management Aims and scope Submit manuscript

Abstract

Hydrothermal carbonization offers the opportunity to reduce the issues related to the management of sewage sludge, enhancing dewaterability and avoiding thermal treatment prior landfill disposal or incineration, as water acts as a subcritical medium which catalyzes the process. The hydrochar obtained can find sustainable application as fuel, sorbent and soil amendment. Here, the effects of activation temperature (550–750 °C), time (1–4 h) and impregnation ratio potassium hydroxide: hydrochar (1–3), as well as their interactions, were investigated by Response Surface Methodology. The carbonaceous sorbent was then applied for the removal of terbuthylazine from aqueous solutions. Solid yields up to 32.31% were obtained, with corresponding ash content ranging from 13.05 to 35.06%. The combined effect of time and temperature significantly affects the ash content. An increase of impregnation ratio or temperature leads to low yields but high terbuthylazine adsorption, while the effect of the activation time on the pollutant removal is negligible. Up to 63.87% of the herbicide was adsorbed by the activated material, at terbuthylazine concentration of 2.5 mg L−1. The developed sorbent well fits the circular economy approach, offering a promising potential for sewage sludge management, as well as for water remediation.

Graphic abstract

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

Access this article

Log in via an institution

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

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3:

Similar content being viewed by others

Abbreviations

AC:

Activated hydrochar

CCD:

Central composite design

DOE:

Design of experiments

HC:

Hydrochar

HTC:

Hydrothermal carbonization

RSM:

Response surface methodology

TBA:

Terbuthylazine

WWTP:

Wastewater treatment plant

References

  1. Yavari S, Malakahmad A, Sapari NB, Yavari S (2017) Sorption properties optimization of agricultural wastes-derived biochars using response surface methodology. Process Saf Environ Prot 109:509–519

    Google Scholar 

  2. Sawai O, Nunoura T, Yamamoto K (2014) Supercritical water gasification of sewage sludge using bench-scale batch reactor: advantages and drawbacks. J Mater Cycles Waste Manag 16:82–92

    Google Scholar 

  3. Huang Y, Yu L, Wang R, Wu J, Takaoka M (2017) Pilot study of intense dewatering of urban sewage sludge. J Mater Cycles Waste Manag 19:88–101

    Google Scholar 

  4. Vouk D, Nakic D, Stirmer N, Cheeseman C (2018) Influence of combustion temperature on the performance of sewage sludge ash as a supplementary cementitious material. J Mater Cycles Waste Manag 20:1458–1467

    Google Scholar 

  5. Cartes J, Neumann P, Hospido A, Vidal G (2018) Life cycle assessment of management alternatives for sludge from sewage treatment plants in Chile: does advanced anaerobic digestion improve environmental performance compared to current practices? J Mater Cycles Waste Manag 20:1530–1540

    Google Scholar 

  6. Yan A, Li J, Liu L, Ma T, Liu J, Ni Y (2018) Centrifugal dewatering of blended sludge from drinking water treatment plant and wastewater treatment plant. J Mater Cycles Waste Manag 20:421–430

    Google Scholar 

  7. Tasca AL, Puccini M, Gori R, Corsi I, Galletti AMR, Vitolo S (2019) Hydrothermal carbonization of sewage sludge: a critical analysis of process severity, hydrochar properties and environmental implications. Waste Manag 93:1–13

    Google Scholar 

  8. dos Reis GS, Wilhelm M, de Silva TCA, Rezwan K, Sampaio CH, Lima EC, de Souza SMAGU (2016) The use of design of experiments for the evaluation of the production of surface rich activated carbon from sewage sludge via microwave and conventional pyrolysis. Appl Therm Eng 93:590–597

    Google Scholar 

  9. Dahhou M, El Moussaouiti M, Arshad MA, Moustahsine S, Assafi M (2018) Synthesis and characterization of drinking water treatment plant sludge-incorporated Portland cement. J Mater Cycles Waste Manag 20:891–901

    Google Scholar 

  10. Genuino DAD, de Luna MDG, Capareda SC (2018) Improving the surface properties of municipal solid waste-derived pyrolysis biochar by chemical and thermal activation: optimization of process parameters and environmental application. Waste Manag 72:255–264

    Google Scholar 

  11. Kim D, Lee K, Bae D, Park KY (2017) Characterizations of biochar from hydrothermal carbonization of exhausted coffee residue. J Mater Cycles Waste Manag 19:1036–1043

    Google Scholar 

  12. Tasca AL, Nessi S, Rigamonti L (2017) Environmental sustainability of agri-food supply chains: an LCA comparison between two alternative forms of production and distribution of endive in northern Italy. J Clean Prod 140:725–741

    Google Scholar 

  13. Yan M, He L, Prabowo B, Fang Z, Lin J, Xu Z, Hu Y (2018) Effect of pressure and atmosphere during hydrothermal treatment on the properties of sewage sludge-derived solid fuel. J Mater Cycles Waste Manag 20:1594–1604

    Google Scholar 

  14. Yan M, Prabowo B, He L, Fang Z, Xu Z, Hu Y (2017) Effect of inorganic coagulant addition under hydrothermal treatment on the dewatering performance of excess sludge with various dewatering conditions. J Mater Cycles Waste Manag 19:1279–1287

    Google Scholar 

  15. Köchermann J, Görsch K, Wirth B, Mühlenberg J, Klemm M (2018) Hydrothermal carbonization: Temperature influence on hydrochar and aqueous phase composition during process water recirculation. J Environ Chem Eng 6:5481–5487

    Google Scholar 

  16. Berge ND, Ro KS, Mao JD, Flora JRV, Chappell MA, Bae SY (2011) Hydrothermal carbonization of municipal waste streams. Environ Sci Technol 45:5696–5703

    Google Scholar 

  17. Hitzl M, Mendez A, Owsianiak M, Renz M (2018) Making hydrochar suitable for agricultural soil: a thermal treatment to remove organic phytotoxic compounds. J Environ Chem Eng 6:7029–7034

    Google Scholar 

  18. Dalias P, Prasad M, Mumme J, Kern J, Stylianou M, Christou A (2018) Low-cost post-treatments improve the efficacy of hydrochar as peat replacement in growing media. J Environ Chem Eng 6:6647–6652

    Google Scholar 

  19. Hnatukova P, Kopecka I, Pivokonsky M (2011) Adsorption of cellular peptides of Microcystis aeruginosa and two herbicides onto activated carbon: effect of surface charge and interactions. Water Res 45:3359–3368

    Google Scholar 

  20. Ormad MP, Miguel N, Claver A, Matesanz JM, Ovelleiro JL (2008) Pesticides removal in the process of drinking water production. Chemosphere 71:97–106

    Google Scholar 

  21. Suciu NA, Ferrari F, Vasileiadis S, Merli A, Capri E, Trevisan M (2013) Pesticides water decontamination in oxygen-limited conditions. J Environ Sci Heal Part B-Pesticides Food Contam Agric Wastes 48:793–799

    Google Scholar 

  22. Sorlini S, Gialdini F, Stefan M (2014) UV/H2O2 oxidation of arsenic and terbuthylazine in drinking water. Environ Monit Assess 186:1311–1316

    Google Scholar 

  23. Tasca AL, Puccini M, Clematis D, Panizza M (2019) Electrochemical removal of terbuthylazine:boron-doped diamond anode coupled with solid polymer electrolyte. Environ Pollut 251:285–291

    Google Scholar 

  24. Quinones DH, Rey A, Alvarez PM, Beltran FJ, Puma GL (2015) Boron doped TiO2 catalysts for photocatalytic ozonation of aqueous mixtures of common pesticides: diuron, o-phenylphenol MCPA and terbuthylazine. Appl Catal B-Environ 178:74–81

    Google Scholar 

  25. Yang H, Wei HQ, Hu LT, Liu HJ, Yang LP, Au CT, Yi B (2016) Mechanism for the photocatalytic transformation of s-triazine herbicides by center dot OH radicals over TiO2. Chem Eng J 300:209–216

    Google Scholar 

  26. Le Cunff J, Tomasic V, Wittine O (2015) Photocatalytic degradation of the herbicide terbuthylazine: preparation, characterization and photoactivity of the immobilized thin layer of TiO2/chitosan. J Photochem Photobiol a-Chem 309:22–29

    Google Scholar 

  27. Alvarez PM, Quinones DH, Terrones I, Rey A, Beltran FJ (2016) Insights into the removal of terbuthylazine from aqueous solution by several treatment methods. Water Res 98:334–343

    Google Scholar 

  28. Salman JM (2014) Optimization of preparation conditions for activated carbon from palm oil fronds using response surface methodology on removal of pesticides from aqueous solution. Arab J Chem 7:101–108

    Google Scholar 

  29. Salman JM, Njoku VO, Hameed BH (2011) Adsorption of pesticides from aqueous solution onto banana stalk activated carbon. Chem Eng J 174:41–48

    Google Scholar 

  30. Gobi K, Mashitah MD, Vadivelu VM (2011) Adsorptive removal of Methylene Blue using novel adsorbent from palm oil mill effluent waste activated sludge: Equilibrium, thermodynamics and kinetic studies. Chem Eng J 171:1246–1252

    Google Scholar 

  31. Zaini MAA, Zakaria M, Mohd-Setapar SH, Che-Yunus MA (2013) Sludge-adsorbents from palm oil mill effluent for methylene blue removal. J Environ Chem Eng 1:1091–1098

    Google Scholar 

  32. Lee XJ, Lee LY, Hiew BYZ, Gan S, Thangalazhy-Gopakumar S, Kiat Ng H (2017) Multistage optimizations of slow pyrolysis synthesis of biochar from palm oil sludge for adsorption of lead. Bioresour Technol 245:944–953

    Google Scholar 

  33. Kacan E (2016) Optimum BET surface areas for activated carbon produced from textile sewage sludges and its application as dye removal. J Environ Manage 166:116–123

    Google Scholar 

  34. Deng H, Zhang G, Xu X, Tao G, Dai J (2010) Optimization of preparation of activated carbon from cotton stalk by microwave assisted phosphoric acid-chemical activation. J Hazard Mater 182:217–224

    Google Scholar 

  35. Zhou N, Chen H, Xi J, Yao D, Zhou Z, Tian Y, Lu X (2017) Biochars with excellent Pb(II) adsorption property produced from fresh and dehydrated banana peels via hydrothermal carbonization. Bioresour Technol 232:204–210

    Google Scholar 

  36. Hoseinzadeh Hesas R, Arami-Niya A, Wan Daud WMA, Sahu JN (2013) Comparison of oil palm shell-based activated carbons produced by microwave and conventional heating methods using zinc chloride activation. J Anal Appl Pyrolysis 104:176–184

    Google Scholar 

  37. Wang X, Zhu N, Yin B (2008) Preparation of sludge-based activated carbon and its application in dye wastewater treatment. J Hazard Mater 153:22–27

    Google Scholar 

  38. Puccini M, Stefanelli E, Tasca AL, Vitolo S (2018) Pollutant removal from gaseous and aqueous phases using hydrochar-based activated carbon. Chem Eng Trans 67:637–642

    Google Scholar 

  39. Smith KM, Fowler GD, Pullket S, Graham NJD (2009) Sewage sludge-based adsorbents: a review of their production, properties and use in water treatment applications. Water Res 43:2569–2594

    Google Scholar 

  40. Ahmadpour A, Do DD (1997) The preparation of activated carbon from macadamia nutshell by chemical activation. Carbon N Y 35:1723–1732

    Google Scholar 

  41. Podstawczyk D, Witek-Krowiak A, Dawiec A, Bhatnagar A (2015) Biosorption of copper(II) ions by flax meal: empirical modeling and process optimization by response surface methodology (RSM) and artificial neural network (ANN) simulation. Ecol Eng 83:364–379

    Google Scholar 

  42. Sabio E, Álvarez-Murillo A, Román S, Ledesma B (2016) Conversion of tomato-peel waste into solid fuel by hydrothermal carbonization: influence of the processing variables. Waste Manag 47:122–132

    Google Scholar 

  43. Ghorbani F, Younesi H, Ghasempouri SM, Zinatizadeh AA, Amini M, Daneshi A (2008) Application of response surface methodology for optimization of cadmium biosorption in an aqueous solution by Saccharomyces cerevisiae. Chem Eng J 145:267–275

    Google Scholar 

  44. Sun Y, Yang G, Zhang L, Sun Z (2017) Preparation of high performance H2S removal biochar by direct fluidized bed carbonization using potato peel waste. Process Saf Environ Prot 107:281–288

    Google Scholar 

  45. Tasca AL, Clematis D, Panizza M, Vitolo S, Puccini M (2019) Herbicide removal from water: investigating the potential of electrochemistry and hydrochar-based activated carbon. Chem Eng Trans 74:841–846

    Google Scholar 

  46. Puccini M, Stefanelli E, Hiltz M, Seggiani M (2017) Activated carbon from hydrochar produced by hydrothermal carbonization of wastes. Chem Eng Trans 57:169–174

    Google Scholar 

  47. Ronix A, Pezoti O, Souza LS, Souza IPAF, Bedin KC, Souza PSC, Silva TL, Melo SAR, Cazetta AL, Almeida VC (2017) Hydrothermal carbonization of coffee husk: optimization of experimental parameters and adsorption of methylene blue dye. J Environ Chem Eng 5:4841–4849

    Google Scholar 

  48. Khoshbouy R, Takahashi F, Yoshikawa K (2019) Preparation of high surface area sludge-based activated hydrochar via hydrothermal carbonization and application in the removal of basic dye. Environ Res 175:457–467

    Google Scholar 

  49. Sevilla M, Fuertes AB (2009) The production of carbon materials by hydrothermal carbonization of cellulose. Carbon N Y 47:2281–2289

    Google Scholar 

  50. Salak Asghari F, Yoshida H (2006) Acid-catalyzed production of 5-hydroxymethyl furfural from d -fructose in subcritical water. Ind Eng Chem Res 45:2163–2173

    Google Scholar 

  51. Saqib NU, Oh M, Jo W, Park S-K, Lee J-Y (2017) Conversion of dry leaves into hydrochar through hydrothermal carbonization (HTC). J Mater Cycles Waste Manag 19:111–117

    Google Scholar 

  52. Zhang JH, Lin QM, Zhao XR (2014) The Hydrochar characters of municipal sewage sludge under different hydrothermal temperatures and durations. J Integr Agric 13:471–482

    Google Scholar 

  53. He C, Giannis A, Wang J-Y (2013) Conversion of sewage sludge to clean solid fuel using hydrothermal carbonization: hydrochar fuel characteristics and combustion behavior. Appl Energy 111:257–266

    Google Scholar 

  54. Marrugo GD, Silgado KJ, Puello J (2015) Adsorption of Cr (VI) by activated carbon from oil palm endocarp: adsorption isotherm and kinetic analysis. Chem Eng Trans 43:613–618

    Google Scholar 

  55. Adinata D, Wan Daud W, Aroua M (2007) Preparation and characterization of activated carbon from palm shell by chemical activation with K2CO3. Bioresour Technol 98:145–149

    Google Scholar 

  56. Sudaryanto Y, Hartono SB, Irawaty W, Hindarso H, Ismadji S (2006) High surface area activated carbon prepared from cassava peel by chemical activation. Bioresour Technol 97:734–739

    Google Scholar 

  57. Kirschhöfer F, Sahin O, Becker GC, Meffert F, Nusser M, Anderer G, Kusche S, Klaeusli T, Kruse A, Brenner-Weiss G (2016) Wastewater treatment—adsorption of organic micropollutants on activated HTC-carbon derived from sewage sludge. Water Sci Technol 73:607–616

    Google Scholar 

  58. Tasca AL, Fletcher AJ, Ghajeri F, Alejandro FM, Palomino GT (2019) Organics adsorption on novel amorphous silica and silica xerogels: microcolumn rapid breakthrough test coupled with sequential injection analysis. J Porous Media 22:1001–1014

    Google Scholar 

  59. Zogorski JS, Faust SD, Haas JH Jr (1976) The kinetics of adsorption of phenols by granular activated carbon. J Colloid Interface Sci 55:329–341

    Google Scholar 

  60. Han L, Ro KS, Sun K, Sun H, Wang Z, Libra JA, Xing B (2016) New evidence for high sorption capacity of hydrochar for hydrophobic organic pollutants. Environ Sci Technol 50:13274–13282

    Google Scholar 

  61. Oehlert GW (2000) A first course in design and analysis of experiments. W H Freeman & Co, Ed., New York (ISBN 0-7167-3510-5)

    Google Scholar 

Download references

Acknowledgements

This work was supported by the project SLUDGE 4.0, funded by Regione Toscana.

Author information

Authors and Affiliations

  1. Department of Civil and Industrial Engineering, University of Pisa, Largo Lucio Lazzarino, 56122, Pisa, Italy

    Andrea Luca Tasca, Monica Puccini, Eleonora Stefanelli & Sandra Vitolo

  2. Department of Civil and Environmental Engineering, University of Florence, via S. Marta 3, 50139, Florence, Italy

    Riccardo Gori

  3. Department of Chemistry and Industrial Chemistry, University of Pisa, Via G. Moruzzi, 13, 56124, Pisa, Italy

    Anna Maria Raspolli Galletti

Authors
  1. Andrea Luca Tasca
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Monica Puccini
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Eleonora Stefanelli
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Riccardo Gori
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Anna Maria Raspolli Galletti
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Sandra Vitolo
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Monica Puccini.

Additional information

Publisher's Note

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

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 959 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Tasca, A.L., Puccini, M., Stefanelli, E. et al. Investigating the activation of hydrochar from sewage sludge for the removal of terbuthylazine from aqueous solutions. J Mater Cycles Waste Manag 22, 1539–1551 (2020). https://doi.org/10.1007/s10163-020-01045-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10163-020-01045-y

Keywords

Search

Navigation