Effect of advanced oxidation processes on the micropollutants and the effluent organic matter contained in municipal wastewater previously treated by three different secondary methods

In this study, wastewater from the output of three different secondary treatment facilities (Activated Sludge, Moving Bed Bioreactor and Coagulation-Flocculation) present in the municipal wastewater treatment plant of Vidy, Lausanne (Switzerland), was further treated with various oxidation processes (UV, UV/H2O2, solar irradiation, Fenton, solar photo-Fenton), at laboratory scale. For this assessment, 6 organic micropollutants in agreement with the new environmental legislation requirements in Switzerland were selected (Carbamazepine, Clarithromycin, Diclofenac, Metoprolol, Benzotriazole, Mecoprop) and monitored throughout the treatment. Also, the overall removal of the organic load was assessed. After each secondary treatment, the efficiency of the AOPs increased in the following order: Coagulation-Flocculation < Activated Sludge < Moving Bed Bioreactor, in almost all cases. From the different combinations tested, municipal wastewater subjected to biological treatment followed by UV/ H2O2 resulted in the highest elimination levels. Wastewater previously treated by physicochemical treatment demonstrated considerably inhibited micropollutant degradation rates. The degradation kinetics were determined, yielding: k (UV) < k (UV/H2O2) and k (Fenton) < k (solar irradiation) < k (photo-Fenton). Finally, the evolution of global pollution parameters (COD & TOC elimination) was followed and the degradation pathways for the effluent organic matter are discussed.

Micropollutant degradation, bacterial inactivation and regrowth risk in wastewater effluents: Influence of the secondary (pre)treatment on the efficiency of Advanced Oxidation Processes

Luiz Felippe De Alencastro, Stefanos Giannakis, Dominique Grandjean, Anoys Magnet, César Pulgarin

In this work, disinfection by 5 Advanced Oxidation Processes was preceded by 3 different secondary treatment systems present in the wastewater treatment plant of Vidy, Lausanne (Switzerland). 5 AOPs after two biological treatment methods (conventional activated sludge and moving bed bioreactor) and a physiochemical process (coagulation-flocculation) were tested in laboratory scale. The dependence among AOPs efficiency and secondary (pre)treatment was estimated by following the bacterial con- centration i) before secondary treatment, ii) after the different secondary treatment methods and iii) after the various AOPs. Disinfection and post-treatment bacterial regrowth were the evaluation in- dicators. The order of efficiency was Moving Bed Bioreactor > Activated Sludge > Coagulation- Flocculation > Primary Treatment. As far as the different AOPs are concerned, the disinfection kinetics were: UVC/H2O2 > UVC and solar photo-Fenton > Fenton or solar light. The contextualization and parallel study of microorganisms with the micropollutants of the effluents revealed that higher exposure times were necessary for complete degradation compared to microorganisms for the UV-based processes and inversed for the Fenton-related ones. Nevertheless, in the Fenton-related systems, the nominal 80% removal of micropollutants deriving from the Swiss legislation, often took place before the elimination of bacterial regrowth risk.

Elsevier2016

Enhancing the photo-Fenton treatment of contaminated water by use of ultrasound and iron-complexing agents

Stefanos Papoutsakis

The photo-Fenton process is a promising emerging technology for the treatment of contaminated water streams. It is based on the generation of reactive oxygen species that are capable of destroying recalcitrant contaminants otherwise unaffected by conventional municipal wastewater treatment method. Among its innate advantages are that it can be catalyzed naturally by solar radiation and the main reagents required are iron and hydrogen peroxide, both abundant and relatively cheap. There are however some important limitations. The process functions best at acidic pH, is negatively affected by some inorganic ions present in natural water and the water requires pH neutralization and iron recuperation following the treatment. These limitations inhibit the application of the process at larger-scale. This work is an attempt to develop new strategies for enhancing the photo-Fenton process for making it a more attractive option for the treatment of municipal or industrial wastewaters. Two main pathways are investigated, the use of ultrasound and the use of iron-complexing agents. Ultrasonic processes have been shown to improve degradation kinetics when applied in combination with photo-Fenton, while at the same time are not as negatively affected by some of the inorganic ions present in water. Iron-complexing agents can maintain iron soluble at a wider operational pH and can also improve process efficiency via pathways discussed at length in the text. Chapter 2 is focused on the application of ultrasound in combination with photo-Fenton for two very distinct applications: 1) A pilot-scale ultrasound/photo-Fenton system was set-up and evaluated for the treatment of three different contaminants with distinct physicochemical properties and at different concentrations. Synergy was evaluated in terms of degradation kinetics and H2O2 consumption efficiency. 2) Ultrasound was applied alone and in combination with photo-Fenton for the treatment of the iodinated contrast agent Iohexol. These agents are injected in patients during radiographic procedures and excreted via urine. This provided an opportunity to examine if ultrasound could improve their treatment in such a complex aquatic medium. Treatment options both in urine (at the source) and in the context of municipal wastewater are discussed. Chapter 3 is focused on the use of EDDS as an iron-complexing agent for degrading contaminants at near neutral pH across a concentration range usually found in different wastewaters (from ÎŒg L-1 to mg L-1 ). EDDS was used both for the treatment of microcontaminants (ÎŒg L-1) in municipal wastewater treatment plant effluents as well as for highly contaminated ( several mg L-1) water. The importance of several factors and operational conditions is discussed. Chapter 4 discusses the possibility of exploiting natural iron-complexing agents (mainly phenolic/polyphenolic compounds) that can be found in some types of wastewater (e.g from natural products processing industries). The concept of reusing polyphenol-rich wastewater in small quantities as an alternative to artificial complexing agents is introduced. As a case study, water containing highly concentrated cork bark extracts (Cork Boiling Wastewater) has been added in natural water spiked with one or several contaminants. Its capacity to maintain Fe3+ soluble at near-neutral pH as well as the effect on Fenton/photo-Fenton degradation were observed.

EPFL2016

Solar photo-Fenton and UV/H2O2 processes against the antidepressant Venlafaxine in urban wastewaters and human urine. Intermediates formation and biodegradability assessment

Luiz Felippe De Alencastro, Stefanos Giannakis, Hubert Girault, Dominique Grandjean, Idriss Hendaoui, Milica Jovic, César Pulgarin

In this work, the use of Advanced Oxidation Processes (AOPs) against the degradation of an emerging contaminant has been subjected under systematic investigation. The optimization of treatment of the anti- depressant drug Venlafaxine (VFA) was performed, using UV light, the combined UV/H2O2 process, solar light, Fenton and finally the solar photo-Fenton process in laboratory scale. The degradation kinetics, the time necessary to remove 90% of the contaminant and the optimal reactants concentration were proposed. The treatment in pure water, (synthetic) wastewater and urine was assessed, in an effort to identify the opportunities and pitfalls the application of process would encounter in a field application. Treatment by the UV-based methods was found sufficiently efficient and the application of the solar photo-Fenton process showed feasibility in a potential field application with appropriate context. Real urban wastewater effluents after biological and physicochemical treatment were tested, as well as human urine, as a proposal for on-site collection and treatment was also treated. Biological treatment before applying the tested AOPs improved their efficiency, and the strategy of diluting urine prior to treatment greatly enhanced the efficacy of the process. Finally, the identification of the degradation pathway and the biodegradability tests of AOPs treated VFA solutions exhibit promising results concerning the strategy of treatment for similar pollutants of emerging concern.

Elsevier Science Sa2017

Enhancing the photo-Fenton treatment of contaminated water by use of ultrasound and iron-complexing agents

Stefanos Papoutsakis

EPFL2016