Upcycling spent brewery grains through the production of carbon adsorbents—application to the removal of carbamazepine from water

Abstract

Spent brewery grains, a by-product of the brewing process, were used as precursor of biochars and activated carbons to be applied to the removal of pharmaceuticals from water. Biochars were obtained by pyrolysis of the raw materials, while activated carbons were produced by adding a previous chemical activation step. The influence of using different precursors (from distinct fermentation processes), activating agents (potassium hydroxide, sodium hydroxide, and phosphoric acid), pyrolysis temperatures, and residence times was assessed. The adsorbents were physicochemically characterized and applied to the removal of the antiepileptic carbamazepine from water. Potassium hydroxide activation produced the materials with the most promising properties and adsorptive removals, with specific surface areas up to 1120 m2 g−1 and maximum adsorption capacities up to 190 ± 27 mg g−1 in ultrapure water. The adsorption capacity suffered a reduction of < 70% in wastewater, allowing to evaluate the impact of realistic matrices on the efficiency of the materials.

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

Fig. 1
Fig. 2
Fig. 3

References

  1. Aga, D.S., 2008. Fate of pharmaceuticals in the environment and in water treatment systems.

    Google Scholar 

  2. Azargohar R, Dalai AK (2008) Steam and KOH activation of biochar: experimental and modeling studies. Microporous Mesoporous Mater 110:413–421. https://doi.org/10.1016/j.micromeso.2007.06.047

    CAS  Article  Google Scholar 

  3. Bahlmann A, Carvalho JJ, Weller MG, Panne U, Schneider RJ (2012) Immunoassays as high-throughput tools: monitoring spatial and temporal variations of carbamazepine, caffeine and cetirizine in surface and wastewaters. Chemosphere 89:1278–1286. https://doi.org/10.1016/j.chemosphere.2012.05.020

    CAS  Article  Google Scholar 

  4. Barrozo MAS, Borel LD, Lira TS, Ataíde CH (2019) Fluid dynamics analysis and pyrolysis of brewer’s spent grain in a spouted bed reactor. Particuology 42:199–207. https://doi.org/10.1016/j.partic.2018.06.001

    CAS  Article  Google Scholar 

  5. Borel LD, Lira TS, Ribeiro JA, Ataíde CH, Barrozo MAS (2018) Pyrolysis of brewer’s spent grain: kinetic study and products identification. Ind Crop Prod 121:388–395. https://doi.org/10.1016/j.indcrop.2018.05.051

    CAS  Article  Google Scholar 

  6. Calisto V, Domingues MRM, Erny GL, Esteves VI (2011) Direct photodegradation of carbamazepine followed by micellar electrokinetic chromatography and mass spectrometry. Water Res 45:1095–1104. https://doi.org/10.1016/j.watres.2010.10.037

    CAS  Article  Google Scholar 

  7. Calisto V, Ferreira CIA, Santos SM, Gil MV, Otero M, Esteves VI (2014) Production of adsorbents by pyrolysis of paper mill sludge and application on the removal of citalopram from water. Bioresour Technol 166:335–344. https://doi.org/10.1016/j.biortech.2014.05.047

    CAS  Article  Google Scholar 

  8. Calisto V, Ferreira CIA, Oliveira JABP, Otero M, Esteves VI (2015) Adsorptive removal of pharmaceuticals from water by commercial and waste-based carbons. J Environ Manag 152:83–90. https://doi.org/10.1016/j.jenvman.2015.01.019

    CAS  Article  Google Scholar 

  9. Calisto V, Jaria G, Silva CP, Ferreira CIA, Otero M, Esteves VI (2017) Single and multi-component adsorption of psychiatric pharmaceuticals onto alternative and commercial carbons. J Environ Manag 192:15–24

    CAS  Article  Google Scholar 

  10. Chen D, Xie S, Chen C, Quan H, Hua L, Luo X, Guo L (2017) Activated biochar derived from pomelo peel as a high-capacity sorbent for removal of carbamazepine from aqueous solution. RSC Adv 7:54969–54979. https://doi.org/10.1039/C7RA10805B

    CAS  Article  Google Scholar 

  11. Clara M, Strenn B, Kreuzinger N (2004) Carbamazepine as a possible anthropogenic marker in the aquatic environment: investigations on the behaviour of carbamazepine in wastewater treatment and during groundwater infiltration. Water Res 38:947–954

    CAS  Article  Google Scholar 

  12. Coates J (2000) Interpretation of infrared spectra-a practical approach. In: Meyers RA (ed) Encyclopedia of Analytical Chemistry. John Wiley & Sons Ltd, Chichester, pp 10815–10837

    Google Scholar 

  13. Delgado N, Capparelli A, Navarro A, Marino D (2019) Pharmaceutical emerging pollutants removal from water using powdered activated carbon: study of kinetics and adsorption equilibrium. J Environ Manag 236:301–308. https://doi.org/10.1016/J.JENVMAN.2019.01.116

    CAS  Article  Google Scholar 

  14. Fekadu S, Alemayehu E, Dewil R, Van der Bruggen B (2019) Pharmaceuticals in freshwater aquatic environments: a comparison of the African and European challenge. Sci Total Environ 654:324–337. https://doi.org/10.1016/J.SCITOTENV.2018.11.072

    CAS  Article  Google Scholar 

  15. Ferraz AI, Tavares MT, Teixeira JA (2005) Sorption of Cr ( III ) from aqueous solutions by spent brewery grain. CHEMPOR 2005 - 9th Int. Chem. Eng. Conf. s.n.

  16. Fontana KB, Chaves ES, Sanchez JDS, Watanabe ERLR, Pietrobelli JMTA, Lenzi GG (2016) Textile dye removal from aqueous solutions by malt bagasse: isotherm, kinetic and thermodynamic studies. Ecotoxicol Environ Saf 124:329–336. https://doi.org/10.1016/j.ecoenv.2015.11.012

    CAS  Article  Google Scholar 

  17. Fontana IB, Peterson M, Cechinel MAP (2018) Application of brewing waste as biosorbent for the removal of metallic ions present in groundwater and surface waters from coal regions. J Environ Chem Eng 6:660–670. https://doi.org/10.1016/J.JECE.2018.01.005

    CAS  Article  Google Scholar 

  18. Freundlich H (1906) Over the adsorption in solution. J Phys Chem 18:385–470

    Google Scholar 

  19. Gonçalves G d C, Nakamura PK, Furtado DF, Veit MT (2017) Utilization of brewery residues to produces granular activated carbon and bio-oil. J Clean Prod 168:908–916. https://doi.org/10.1016/J.JCLEPRO.2017.09.089

    Article  Google Scholar 

  20. Ho YS, McKay G, Wase DAJ, Forster CF (2000) Study of the sorption of divalent metal ions on to peat. Adsorpt Sci Technol 18:639–650. https://doi.org/10.1260/0263617001493693

    CAS  Article  Google Scholar 

  21. Hunsom M, Autthanit C (2013) Adsorptive purification of crude glycerol by sewage sludge-derived activated carbon prepared by chemical activation with H3PO4 , K2CO3 and KOH. Chem Eng J 229:334–343. https://doi.org/10.1016/j.cej.2013.05.120

    CAS  Article  Google Scholar 

  22. Jaria G, Calisto V, Gil MV, Otero M, Esteves VI (2015) Removal of fluoxetine from water by adsorbent materials produced from paper mill sludge. J Colloid Interface Sci 448:32–40. https://doi.org/10.1016/j.jcis.2015.02.002

    CAS  Article  Google Scholar 

  23. Jaria G, Silva CP, Ferreira CIA, Otero M, Calisto V (2017) Sludge from paper mill effluent treatment as raw material to produce carbon adsorbents: an alternative waste management strategy. J Environ Manag 188:203–211

    CAS  Article  Google Scholar 

  24. Jaria G, Calisto V, Silva CP, Gil MV, Otero M, Esteves VI (2019) Obtaining granular activated carbon from paper mill sludge – A challenge for application in the removal of pharmaceuticals from wastewater. Sci Total Environ 653:393–400. https://doi.org/10.1016/J.SCITOTENV.2018.10.346

    CAS  Article  Google Scholar 

  25. Jelic A, Gros M, Ginebreda A, Cespedes-Sánchez R, Ventura F, Petrovic M, Barcelo D (2011) Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment. Water Res 45:1165–1176. https://doi.org/10.1016/j.watres.2010.11.010

    CAS  Article  Google Scholar 

  26. Jones OA, Voulvoulis N, Lester JN (2002) Aquatic environmental assessment of the top 25 English prescription pharmaceuticals. Water Res 36:5013–5022

    CAS  Article  Google Scholar 

  27. Lagergren S (1898) About the theory of so-called adsorption of soluble substances. K Sven Vetenskapsakademiens 24:1–39

    Google Scholar 

  28. Langmuir I (1916) The constitution and fundamental properties of solids and liquids. J Am Chem Soc 38:2221–2295. https://doi.org/10.1021/ja02268a002

    CAS  Article  Google Scholar 

  29. Li WCC (2014) Occurrence, sources, and fate of pharmaceuticals in aquatic environment and soil. Environ Pollut 187:193–201. https://doi.org/10.1016/j.envpol.2014.01.015

    CAS  Article  Google Scholar 

  30. Mahmood T, Ali R, Naeem A, Hamayun M, Aslam M (2017) Potential of used Camellia sinensis leaves as precursor for activated carbon preparation by chemical activation with H3PO4; optimization using response surface methodology. Process Saf Environ Prot 109:548–563. https://doi.org/10.1016/j.psep.2017.04.024

    CAS  Article  Google Scholar 

  31. Molina-Sabio M, Rodríguez-Reinoso F, Caturla F, Sellés MJ (1995) Porosity in granular carbons activated with phosphoric acid. Carbon N Y 33:1105–1113. https://doi.org/10.1016/0008-6223(95)00059-M

    CAS  Article  Google Scholar 

  32. Nielsen L, Zhang P, Bandosz TJ (2015) Adsorption of carbamazepine on sludge/fish waste derived adsorbents: effect of surface chemistry and texture. Chem Eng J 267:170–181. https://doi.org/10.1016/J.CEJ.2014.12.113

    CAS  Article  Google Scholar 

  33. Olajire A, Abidemi J, Lateef A, Benson NU (2017) Adsorptive desulphurization of model oil by Ag nanoparticles-modified activated carbon prepared from brewer’s spent grains. J Environ Chem Eng 5:147–159. https://doi.org/10.1016/j.jece.2016.11.033

    CAS  Article  Google Scholar 

  34. Oliveira G, Calisto V, Santos SM, Otero M, Esteves VI (2018) Paper pulp-based adsorbents for the removal of pharmaceuticals from wastewater: a novel approach towards diversification, vol 631–632, pp 1018–1028

    Google Scholar 

  35. Olszewski MP, Arauzo PJ, Wądrzyk M, Kruse A (2019) Py-GC-MS of hydrochars produced from brewer’s spent grains. J Anal Appl Pyrolysis 140:255–263. https://doi.org/10.1016/j.jaap.2019.04.002

    CAS  Article  Google Scholar 

  36. Silva JP, Sousa S, Rodrigues J, Antunes H, Porter J, Gonçalves I, Ferreira-Dias S (2004) Adsorption of acid orange 7 dye in aqueous solutions by spent brewery grains. Sep Purif Technol 40:309–315. https://doi.org/10.1016/j.seppur.2004.03.010

    CAS  Article  Google Scholar 

  37. Silva CP, Jaria G, Otero M, Esteves VI, Calisto V (2019) Adsorption of pharmaceuticals from biologically treated municipal wastewater using paper mill sludge-based activated carbon. Environ Sci Pollut Res 26:13173–13184. https://doi.org/10.1007/s11356-019-04823-w

    CAS  Article  Google Scholar 

  38. Sips R (1948) On the structure of a catalyst surface. J Chem Phys 16:490–495. https://doi.org/10.1063/1.1746922

    CAS  Article  Google Scholar 

  39. To M-H, Hadi P, Hui C-W, Lin CSK, McKay G (2017) Mechanistic study of atenolol, acebutolol and carbamazepine adsorption on waste biomass derived activated carbon. J Mol Liq 241:386–398. https://doi.org/10.1016/J.MOLLIQ.2017.05.037

    CAS  Article  Google Scholar 

  40. Torrellas SÁ, García Lovera R, Escalona N, Sepúlveda C, Sotelo JL, García J (2015) Chemical-activated carbons from peach stones for the adsorption of emerging contaminants in aqueous solutions. Chem Eng J 279:788–798

    CAS  Article  Google Scholar 

  41. Tran NH, Reinhard M, Gin KY-H (2018) Occurrence and fate of emerging contaminants in municipal wastewater treatment plants from different geographical regions-a review. Water Res 133:182–207. https://doi.org/10.1016/J.WATRES.2017.12.029

    CAS  Article  Google Scholar 

  42. Vanreppelen K, Vanderheyden S, Kuppens T, Schreurs S, Yperman J, Carleer R (2014) Activated carbon from pyrolysis of brewer’s spent grain: production and adsorption properties. Waste Manag Res 32:634–645. https://doi.org/10.1177/0734242X14538306

    CAS  Article  Google Scholar 

  43. Wierzba S, Andrzej K (2019) Heavy metal sorption in biosorbents-using spent grain from the brewing industry. J Clean Prod 225:112–120. https://doi.org/10.1016/j.jclepro.2019.03.286

    CAS  Article  Google Scholar 

  44. Wierzba S, Rajfur M, Nabrdalik M, Kłos A (2019) Assessment of the influence of counter ions on biosorption of copper cations in brewer’s spent grain-waste product generated during beer brewing process. Microchem J 145:196–203. https://doi.org/10.1016/j.microc.2018.10.040

    CAS  Article  Google Scholar 

Download references

Acknowledgments

The authors would like to thank Valdemar Esteves, Marta Otero, and Guilaine Jaria for the helpful scientific discussions. Milton Fontes and workers of Aveiro’s Sewage Treatment Plant (Águas do Centro Litoral) are gratefully acknowledged for assistance on the effluent sampling campaigns. The authors also thank Faustino Microcervejeira, Lda. (Aveiro, Portugal) and its head brewer Gonçalo Faustino for kindly providing the brewing residues used in this work.

Funding

Thanks are due for the financial support to CESAM (UID/AMB/50017/2019), to FCT/MEC through national funds, and the co-funding by the FEDER, within the PT2020 Partnership Agreement and Compete 2020. Vânia Calisto is thankful to FCT for the Scientific Employment Stimulus Program (CEECIND/00007/2017), while María V. Gil acknowledges support from a Ramón y Cajal grant (RYC-2017-21937) of the Spanish government, co-financed by the European Social Fund (ESF).

Author information

Affiliations

Authors

Corresponding author

Correspondence to Vânia Calisto.

Additional information

Publisher’s note

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

Responsible editor: Tito Roberto Cadaval Jr

Electronic supplementary material

ESM 1

E-supplementary data of this work can be found in online version of the paper. (PDF 1.24 mb)

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Sousa, A.F.C., Gil, M.V. & Calisto, V. Upcycling spent brewery grains through the production of carbon adsorbents—application to the removal of carbamazepine from water. Environ Sci Pollut Res (2020). https://doi.org/10.1007/s11356-020-09543-0

Download citation

Keywords

  • Brewery wastes
  • Pyrolysis
  • Chemical activation
  • Activated carbon
  • Pharmaceuticals
  • Wastewater treatment