A tubular ceramic membrane coated with TiO2-P25 for radial addition of H2O2 towards AMX removal from synthetic solutions and secondary urban wastewater

Diório, Alexandre; Díaz-Angulo, Jennyfer; Castellanos, Reynel M.; Gomes, Ana I.; Bergamasco, Rosângela; Vieira, Marcelo Fernandes; Dezotti, Márcia; Mueses, Miguel Angel; Machuca-Martinez, Fiderman; Vilar, Vítor J. P.

doi:10.1007/s11356-021-14297-4

A tubular ceramic membrane coated with TiO₂-P25 for radial addition of H₂O₂ towards AMX removal from synthetic solutions and secondary urban wastewater

Occurrence, Impact and Elimination of Contaminants of Emerging Concern (CECs) in Soil, Water and Air Streams: Advances and Challenges in Ibero-American Countries
Published: 13 May 2021

Volume 29, pages 42120–42129, (2022)
Cite this article

Environmental Science and Pollution Research Aims and scope Submit manuscript

Alexandre Diório¹,
Jennyfer Díaz-Angulo²,
Reynel M. Castellanos³,
Ana I. Gomes ORCID: orcid.org/0000-0002-5719-3013⁴,
Rosângela Bergamasco¹,
Marcelo Fernandes Vieira¹,
Márcia Dezotti³,
Miguel Angel Mueses⁵,
Fiderman Machuca-Martinez² &
…
Vítor J. P. Vilar⁴

799 Accesses
3 Citations
Explore all metrics

Abstract

This work aims to integrate several hydrogen peroxide (H₂O₂) activation mechanisms, photolysis (UVC irradiation), chemical electron transfer (TiO₂-P25 photocatalysis), and reaction with TiO₂-P25 in dark conditions, for reactive oxygen species (ROS) generation towards the removal of contaminants of emerging concern (CECs), in a single unit operated in continuous-flow mode. An H₂O₂ stock solution is fed by the lumen side of a tubular ceramic membrane, delivering the oxidant to the (i) catalyst immobilized in the membrane shell-side and (ii) annular reaction zone (ARZ, space between membrane shell-side and outer quartz tube) where CECs contaminated water flows with a helix trajectory, being activated by UV light provided by four lamps placed symmetrically around the reactor. First, the effect of several parameters in the removal of a CEC target molecule, amoxicillin (AMX), was evaluated using a synthetic solution ([AMX]_inlet = 2.0 mg L^-1): (i) light source (UVA or UVC radiation), (ii) H₂O₂ dose, (iii) H₂O₂ injection method (radial permeation vs. upstream injection), and (iv) number of TiO₂-P25 layers deposited on the membrane. The UVC/H₂O₂/TiO₂ system with radial addition of H₂O₂ (20 mg L^-1) and 9-TiO₂-P25 layers provided the highest AMX removal efficiency (72.2 ± 0.5%) with a UV fluence of 45 mJ cm^-2 (residence time of 4.6 s), due to the synergic effect of four mechanisms: (i) AMX photolysis, (ii) H₂O₂ photocleavage, (iii) TiO₂-P25 photoactivation, and (iv) chemical reactions between H₂O₂ and TiO₂-P25. The urban wastewater matrix showed a negative effect on AMX removal (~44%) due to the presence of ROS scavengers and light-filtering species.

Graphical 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

Performance evaluation of a new continuous flow tubular electrochemical reactor with ceramic membrane for the treatment of wastewater

Article 03 July 2023

Hydroxyl radical intensified Cu2O NPs/H2O2 process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer

Article 15 June 2020

State-of-the-art and current challenges for TiO2/UV-LED photocatalytic degradation of emerging organic micropollutants

Article 14 October 2020

Data availability

All data generated or analyzed during this study are included in this article.

References

Anjali R, Shanthakumar S (2019) Insights on the current status of occurrence and removal of antibiotics in wastewater by advanced oxidation processes. J Environ Manag 246:51–62. https://doi.org/10.1016/j.jenvman.2019.05.090
Article CAS Google Scholar
Baeza C, Knappe DRU (2011) Transformation kinetics of biochemically active compounds in low-pressure UV photolysis and UV/H₂O₂ advanced oxidation processes. Water Res 45(15):4531–4543. https://doi.org/10.1016/j.watres.2011.05.039
Article CAS Google Scholar
Cai MJ, Lin YP (2016) Effects of effluent organic matter (EfOM) on the removal of emerging contaminants by ozonation. Chemosphere 151:332–338. https://doi.org/10.1016/j.chemosphere.2016.02.094
Article CAS Google Scholar
Carrera G, Vegué L, Ventura F, Hernández-Valencia A, Devesa R, Boleda MR (2019) Dioxanes and dioxolanes in source waters: occurrence, odor thresholds and behavior through upgraded conventional and advanced processes in a drinking water treatment plant. Water Res 156:404–413. https://doi.org/10.1016/j.watres.2019.03.026
Article CAS Google Scholar
Castellanos RM, Paulo Bassin J, Dezotti M, Boaventura RAR, Vilar VJP (2020) Tube-in-tube membrane reactor for heterogeneous TiO₂ photocatalysis with radial addition of H₂O₂. Chem Eng J 395:124998. https://doi.org/10.1016/j.cej.2020.124998
Article CAS Google Scholar
Cataldo F (2014) Hydrogen peroxide photolysis with different UV light sources including a new UV-LED light source. Front Chem 23:99–110
Google Scholar
Data, Ra, (2019). Amoxicillin market analysis, by infection type, route (oral, intravenous), form (tablets, capsule, suspensions, syrup, powder), distribution channels (hospitals pharmacies, retail pharmacies, online pharmacies, others), region, forecasts to 2026. .
de la Cruz N, Esquius L, Grandjean D, Magnet A, Tungler A, de Alencastro LF, Pulgarín C (2013) Degradation of emergent contaminants by UV, UV/H₂O₂ and neutral photo-Fenton at pilot scale in a domestic wastewater treatment plant. Water Res 47(15):5836–5845. https://doi.org/10.1016/j.watres.2013.07.005
Article CAS Google Scholar
Díaz-Angulo J, Cotillas S, Gomes AI, Miranda SM, Mueses M, Machuca-Martínez F, Rodrigo MA, Boaventura RAR, Vilar VJP (2021) A tube-in-tube membrane microreactor for tertiary treatment of urban wastewaters by photo-Fenton at neutral pH: a proof of concept. Chemosphere 263:128049. https://doi.org/10.1016/j.chemosphere.2020.128049
Article CAS Google Scholar
Elmolla ES, Chaudhuri M (2009) Degradation of the antibiotics amoxicillin, ampicillin and cloxacillin in aqueous solution by the photo-Fenton process. J Hazard Mater 172(2-3):1476–1481. https://doi.org/10.1016/j.jhazmat.2009.08.015
Article CAS Google Scholar
Elmolla ES, Chaudhuri M (2010) Photocatalytic degradation of amoxicillin, ampicillin and cloxacillin antibiotics in aqueous solution using UV/TiO₂ and UV/H₂O₂/TiO₂ photocatalysis. Desalination 252(1-3):46–52. https://doi.org/10.1016/j.desal.2009.11.003
Article CAS Google Scholar
Glaze WH, Kang J, Chapin D (1987) The chemistry of water treatment processes involving ozone, hydrogen peroxide and ultraviolet radiation. Ozone Sci Eng 9:335–352. https://doi.org/10.1080/01919518708552148
Article CAS Google Scholar
Gomes AI, Vilar VJP, Boaventura RAR (2009) Synthetic and natural waters disinfection using solar radiation in a pilot plant with CPCs. Catal Today 144:55–61. https://doi.org/10.1016/j.cattod.2008.12.023
Article CAS Google Scholar
Gomes AI, Soares TF, Silva TFCV, Boaventura RAR, Vilar VJP (2020) Ozone-driven processes for mature urban landfill leachate treatment: organic matter degradation, biodegradability enhancement and treatment costs for different reactors configuration. Sci Total Environ 724:138083. https://doi.org/10.1016/j.scitotenv.2020.138083
Article CAS Google Scholar
Huling SG, Pivetz BE (2006) In-situ chemical oxidation (No. EPA/600/R-06/072). Washington, DC
Google Scholar
Huttner A, Bielicki J, Clements MN, Frimodt-Møller N, Muller AE, Paccaud J-P, Mouton JW (2019) Oral amoxicillin and amoxicillin–clavulanic acid: properties, indications and usage. Clin Microbiol Infect 26:871–879. https://doi.org/10.1016/j.cmi.2019.11.028
Article CAS Google Scholar
Ikehata K, Wang-Staley L, Qu X, Li Y (2016) Treatment of groundwater contaminated with 1,4-dioxane, tetrahydrofuran, and chlorinated volatile organic compounds using advanced oxidation processes. Ozone Sci Eng 38(6):413–424. https://doi.org/10.1080/01919512.2016.1198686
Article CAS Google Scholar
Li X, Chen C, Zhao J (2001) Mechanism of photodecomposition of H₂O₂ on TiO₂ surfaces under visible light irradiation. Langmuir 17(13):4118–4122. https://doi.org/10.1021/la010035s
Article CAS Google Scholar
Li X, Shen T, Wang D, Yue X, Liu X, Yang Q, Cao J, Zheng W, Zeng G (2012) Photodegradation of amoxicillin by catalyzed Fe³⁺/H₂O₂ process. J Environ Sci 24(2):269–275
Article CAS Google Scholar
Liang X, Chen B, Nie X, Shi Z, Huang X, Li X (2013) The distribution and partitioning of common antibiotics in water and sediment of the Pearl River Estuary, South China. Chemosphere 92(11):1410–1416. https://doi.org/10.1016/j.chemosphere.2013.03.044
Article CAS Google Scholar
Liu W, Andrews SA, Stefan MI, Bolton JR (2003) Optimal methods for quenching H₂O₂ residuals prior to UFC testing. Water Res 37(15):3697–3703. https://doi.org/10.1016/S0043-1354(03)00264-1
Article CAS Google Scholar
Lofrano G, Pedrazzani R, Libralato G, Carotenuto M (2017) Advanced oxidation processes for antibiotics removal: a review. Curr Org Chem 21:1–14. https://doi.org/10.2174/1385272821666170103162813
Article CAS Google Scholar
Lumbaque EC, Sirtori C, Vilar VJP (2020) Heterogeneous photocatalytic degradation of pharmaceuticals in synthetic and real matrices using a tube-in-tube membrane reactor with radial addition of H₂O₂. Sci Total Environ 743:140629. https://doi.org/10.1016/j.scitotenv.2020.140629
Article CAS Google Scholar
Matamoros V, Arias CA, Nguyen LX, Salvadó V, Brix H (2012) Occurrence and behavior of emerging contaminants in surface water and a restored wetland. Chemosphere 88(9):1083–1089. https://doi.org/10.1016/j.chemosphere.2012.04.048
Article CAS Google Scholar
Morasch B, Bonvin F, Reiser H, Grandjean D, de Alencastro LF, Perazzolo C, Chèvre N, Kohn T (2010) Occurrence and fate of micropollutants in the Vidy Bay of Lake Geneva, Switzerland. Part II: micropollutant removal between wastewater and raw drinking water. Environ Toxicol Chem 29(8):1658–1668. https://doi.org/10.1002/etc.222
Article CAS Google Scholar
Moreira FC, Soler J, Alpendurada MF, Boaventura RAR, Brillas E, Vilar VJP (2016) Tertiary treatment of a municipal wastewater toward pharmaceuticals removal by chemical and electrochemical advanced oxidation processes. Water Res 105:251–263. https://doi.org/10.1016/j.watres.2016.08.036
Article CAS Google Scholar
Nogueira RFP, Oliveira MC, Paterlini WC (2005) Simple and fast spectrophotometric determination of H₂O₂ in photo-Fenton reactions using metavanadate. Talanta 66(1):86–91. https://doi.org/10.1016/j.talanta.2004.10.001
Article CAS Google Scholar
O’Brien M, Baxendale IR, Ley S v (2010) Flow ozonolysis using a semipermeable Teflon AF-2400 membrane to effect gas - liquid contact. Org Lett 12(7):1596–1598. https://doi.org/10.1021/ol100322t
Article CAS Google Scholar
O'Dowd K, Pillai SC (2020) Photo-Fenton disinfection at near neutral pH: process, parameter optimization and recent advances. J Environ Chem Eng 8(5):104063. https://doi.org/10.1016/j.jece.2020.104063
Article CAS Google Scholar
Olama N, Dehghani M, Malakootian M (2018) The removal of amoxicillin from aquatic solutions using the TiO₂/UV-C nanophotocatalytic method doped with trivalent iron. Appl Water Sci 8(4):97. https://doi.org/10.1007/s13201-018-0733-7
Article CAS Google Scholar
Pignatello JJ, Oliveros E, MacKay A (2006) Advanced oxidation processes for organic contaminant destruction based on the Fenton reaction and related chemistry. Crit Rev Environ Sci Technol 36(1):1–84. https://doi.org/10.1080/10643380500326564
Article CAS Google Scholar
Ramírez-Franco JH, Galeano L-A, Vicente M-A (2019) Fly ash as photo-Fenton catalyst for the degradation of amoxicillin. J Environ Chem Eng 7(5):103274. https://doi.org/10.1016/j.jece.2019.103274
Article CAS Google Scholar
Rivas J, Gimeno O, Borralho T, Sagasti J (2011) UV-C and UV-C/peroxide elimination of selected pharmaceuticals in secondary effluents. Desalination 279(1-3):115–120. https://doi.org/10.1016/j.desal.2011.05.066
Article CAS Google Scholar
Salazar C, Contreras N, Mansilla HD, Yáñez J, Salazar R (2016) Electrochemical degradation of the antihypertensive losartan in aqueous medium by electro-oxidation with boron-doped diamond electrode. J Hazard Mater 319:84–92. https://doi.org/10.1016/j.jhazmat.2016.04.009
Article CAS Google Scholar
Sánchez LD, Taxt-Lamolle SFM, Hole EO, Krivokapić A, Sagstuen E, Haugen HJ (2013) TiO₂ suspension exposed to H₂O₂ in ambient light or darkness: degradation of methylene blue and EPR evidence for radical oxygen species. Appl Catal B-Environ 142-143:662–667. https://doi.org/10.1016/j.apcatb.2013.05.017
Article CAS Google Scholar
Schneider J, Matsuoka M, Takeuchi M, Zhang J, Horiuchi Y, Anpo M, Bahnemann DW (2014) Understanding TiO2 photocatalysis: mechanisms and materials. Chem Rev 114:9919–9986. https://doi.org/10.1021/cr5001892
Article CAS Google Scholar
Serna-Galvis EA, Botero-Coy AM, Martínez-Pachón D, Moncayo-Lasso A, Ibáñez M, Hernández F, Torres-Palma RA (2021) Degradation of seventeen contaminants of emerging concern in municipal wastewater effluents by sonochemical advanced oxidation processes. Water Res 154:349–360. https://doi.org/10.1016/j.watres.2019.01.045
Article CAS Google Scholar
Sirtori C, Zapata A, Gernjak W, Malato S, Lopez A, Agüera A (2011) Solar photo-Fenton degradation of nalidixic acid in waters and wastewaters of different composition. Analytical assessment by LC-TOF-MS. Water Res 45(4):1736–1744. https://doi.org/10.1016/j.watres.2010.11.023
Article CAS Google Scholar
Snyder EM, Pleus RC, Snyder SA (2005) Pharmaceuticals and EDCS in the US water industry - an update. J Am Water Works Assoc 97(11):32–36
Article CAS Google Scholar
Stasinakis AS (2008) Use of selected advanced oxidation processes (AOPs) for wastewater treatment - a mini review. Glob Nest J 10(3):376–385
Google Scholar
Szymański K, Morawski AW, Mozia S (2018) Effectiveness of treatment of secondary effluent from a municipal wastewater treatment plant in a photocatalytic membrane reactor and hybrid UV/H₂O₂ – ultrafiltration system. Chem Eng Process 125:318–324. https://doi.org/10.1016/j.cep.2017.11.015
Article CAS Google Scholar
Vilar VJP, Alfonso-Muniozguren P, Monteiro JP, Lee J, Miranda SM, Boaventura RAR (2020) Tube-in-tube membrane microreactor for photochemical UVC/H₂O₂ processes: a proof of concept. Chem Eng J 379:122341. https://doi.org/10.1016/j.cej.2019.122341
Article CAS Google Scholar
Zhang Q, Li C, Li T (2013) Rapid photocatalytic decolorization of methylene blue using high photon flux UV/TiO₂/H₂O₂ process. Chem Eng J 217:407–413. https://doi.org/10.1016/J.CEJ.2012.11.106
Article CAS Google Scholar
Ziolli RL, Jardim WF (1998) Mecanismo de fotodegradação de compostos orgânicos catalisada por TiO₂. Química Nova 21(3):319–325
Article CAS Google Scholar

Download references

Funding

The financial support of this work is acknowledged: (i) the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior, from Brasil (CAPES), with Finance Code 001; (ii) Associate Laboratory LSRE-LCM (base funding, UIDB/50020/2020), by national funds through FCT/MCTES (PIDDAC); and (iii) Project NOR-WATER funded by INTERREG VA Spain-Portugal cooperation programme, Cross-Border North Portugal/Galiza Spain Cooperation Program (POCTEP). The authors also acknowledge Brazilian Agencies Capes (PROEX 0070041) and FAPERJ (reference E-26/202.994/2015). Reynel M. Castellanos acknowledges his scholarship (141666/2018-8) from CNPq (Brazil), and J. Diaz-Angulo thanks Colciencias-Colombia for her scholarships (647). Vítor J.P. Vilar acknowledges the FCT Individual Call to Scientific Employment Stimulus 2017 (CEECIND/01317/2017).

Author information

Authors and Affiliations

Department of Chemical Engineering, State University of Maringá, Av., Building D-90, CEP 87020-900, Colombo, PR, 5790, Brazil
Alexandre Diório, Rosângela Bergamasco & Marcelo Fernandes Vieira
Escuela de Ingeniería Quimica, Universidad del Valle, A.A, 25360, Cali, Colombia
Jennyfer Díaz-Angulo & Fiderman Machuca-Martinez
Chemical Engineering Program, COPPE, Federal University of Rio de Janeiro, P.O. Box 68502, Rio de Janeiro, RJ, 21941-972, Brazil
Reynel M. Castellanos & Márcia Dezotti
Laboratory of Separation and Reaction Engineering—Laboratory of Catalysis and Materials (LSRE-LCM), Departamento de Engenharia Química, Faculdade de Engenharia da Universidade do Porto, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal
Ana I. Gomes & Vítor J. P. Vilar
Photocatalysis and Solar Photoreactors Engineering, Chemical Engineering Program, Universidad de Cartagena, A.A. 1382–Postal, 195, Cartagena, Colombia
Miguel Angel Mueses

Authors

Alexandre Diório
View author publications
You can also search for this author in PubMed Google Scholar
Jennyfer Díaz-Angulo
View author publications
You can also search for this author in PubMed Google Scholar
Reynel M. Castellanos
View author publications
You can also search for this author in PubMed Google Scholar
Ana I. Gomes
View author publications
You can also search for this author in PubMed Google Scholar
Rosângela Bergamasco
View author publications
You can also search for this author in PubMed Google Scholar
Marcelo Fernandes Vieira
View author publications
You can also search for this author in PubMed Google Scholar
Márcia Dezotti
View author publications
You can also search for this author in PubMed Google Scholar
Miguel Angel Mueses
View author publications
You can also search for this author in PubMed Google Scholar
Fiderman Machuca-Martinez
View author publications
You can also search for this author in PubMed Google Scholar
Vítor J. P. Vilar
View author publications
You can also search for this author in PubMed Google Scholar

Contributions

The statement to specify the contribution of each co-author is as follows:

- Conceived and designed the experiments: Reynel M. Castellanos and Jennyfer Díaz-Angulo

- Performed the experiments: Reynel M. Castellanos and Jennyfer Días-Angulo

- Analyzed the data: Alexandre Diório, Reynel M. Castellanos, Jennyfer Días-Angulo, and Ana I. Gomes

- Contributed reagents/materials/funding: Rosângela Bergamasco, Marcelo Fernandes Vieira, Márcia Dezotti, Miguel Angel Mueses, Fiderman Machuca-Martinez, and Vítor J. P. Vilar

- Drafted or revised the manuscript: Alexandre Diório, Reynel M. Castellanos, Jennyfer Díaz-Angulo, Ana I. Gomes, Rosângela Bergamasco, Marcelo Fernandes Vieira, Márcia Dezotti, Miguel Angel Mueses, Fiderman Machuca-Martinez, and Vítor J. P. Vilar

Corresponding authors

Correspondence to Ana I. Gomes or Vítor J. P. Vilar.

Ethics declarations

Ethics approval and consent to participate

Not applicable.

Consent for publication

Not applicable.

Competing interests

The authors declare no competing interests.

Additional information

Responsible Editor: Philippe Garrigues

This manuscript describes an original work, has not been published before, and is not under consideration by any other journal.

Publisher’s note

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

Highlights

- Low footprint membrane photoreactor able to activate H₂O₂ into ROS;

- The membrane acts as photocatalyst support and oxidant-catalyst/water contactor;

- H₂O₂ activation by energy, chemical electron transfer, and TiO₂-H₂O₂ interaction;

Rights and permissions

Reprints and permissions

About this article

Cite this article

Diório, A., Díaz-Angulo, J., Castellanos, R.M. et al. A tubular ceramic membrane coated with TiO₂-P25 for radial addition of H₂O₂ towards AMX removal from synthetic solutions and secondary urban wastewater. Environ Sci Pollut Res 29, 42120–42129 (2022). https://doi.org/10.1007/s11356-021-14297-4

Download citation