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Ministerio de Universidades - Gobierno de España

Título: ELIMINACIÓN DE XENOBIÓTICOS DE AGUAS RESIDUALES URBANAS MEDIANTE BIORREACTORES DE MEMBRANA SUMERGIDA
Autor: González Pérez, Daniel María
Universidad: Universidad de Granada
Departamento: Ingeniería civil
Fecha de Lectura: 07/07/2017
Programa de doctorado: Programa Oficial de Doctorado en Ingeniería Civil y Arquitectura
Dirección:
- Pérez Pérez, Jorge Ignacio (DIRECTOR)
- GÓMEZ NIETO, MIGUEL ÁNGEL (DIRECTOR)
Tribunal:
- NEBOT SANZ, ENRIQUE (PRESIDENTE)
- Martín Pascual, Jaime (SECRETARIO)
- Muñío Martínez, María del Mar (VOCAL)
- ESPÍNOLA LOZANO, FRANCISCO (VOCAL)
- APARICIO GOMEZ, IRENE (VOCAL)
Descriptores:
- INGENIERIA CIVIL
- ARQUITECTURA
Fichero de tesis:
ISBN: 9788491633860

http://0-hera.ugr.es.adrastea.ugr.es/tesisugr/26754368.pdf

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Resumen:
Resumen La falta de acceso al agua ha sido siempre un factor limitante para el desarrollo de las sociedades y el sostenimiento de los ecosistemas. En regiones donde coinciden unos escasos recursos hídricos con una elevada densidad de población la mejora en la depuración de las aguas residuales y el uso de fuentes no convencionales de agua se presenta como una necesidad. La reutilización de las aguas residuales, permite aumentar los recursos hídricos disponibles a la vez que disminuye el impacto ocasionado por la carga contaminante presente en las aguas residuales. La sociedad moderna depende de gran cantidad de compuestos xenobióticos, los cuales acaban llegando a las aguas residuales presentando estas una mezcla diversa de compuestos xenobióticos habitualmente con bajas concentraciones (¿g/L o ng/L). La eliminación de los xenobióticos en los sistemas de tratamiento de aguas residuales depende de las características del compuesto y de la naturaleza del proceso. Diversos estudios confirman que muchos xenobióticos iii son relativamente eliminados durante los tratamientos convencionales de fangos activos (CASP) sin embargo otros apenas son eliminados y alcanzan las masas de agua a través de los efluentes de EDARs convencionales. Como alternativa se encuentran los biorreactores de membranas sumergida (MBR), basados en el mismo principio biológico de fangos activos que los CASP, realizando la separación sólido-líquido mediante filtración a través de una membrana. La tecnología MBR se ha mostrado eficaz en la eliminación de materia orgánica disuelta, reducción de nitrógeno y desinfección física de las aguas residuales. Por otro lado, los mecanismos por los cuales son parcialmente eliminados los diferentes xenobióticos mediante sistemas de fangos activos son la biotransformación o biodegradación, la volatilización o la adsorción sobre fango, dependiendo de la naturaleza del compuesto. Determinadas variables del proceso biológico como el tiempo de retención celular (SRT) y el tiempo de retención hidráulico (HRT) afectan a la eliminación de estas sustancias, y los MBRs presentan mayores valores que los CASP para estos parámetros, pudiendo representar una interesante opción para su eliminación. Los xenobióticos se pueden diferenciar entre los considerados como contaminantes clásicos, sobre los que existe preocupación por su presencia en el medio acuático y los efectos que ello acarrea desde hace años, y los contaminantes emergentes, cuyos efectos en el medio ambiente han comenzado a suscitar inquietud en los últimos años. El presente trabajo pretende valorar la eficacia de la tecnología MBR en la eliminación de xenobióticos de las aguas residuales urbanas bajo condiciones de elevado tiempo de retención celular (SRT) y elevado tiempo de retención hidráulica (HRT), y para el desarrollo del mismo se seleccionaron dos de los grupos de xenobióticos más importantes, los fármacos entre los considerados contaminantes emergentes y los hidrocarburos aromáticos policíclicos entre los contaminantes clásicos. Dada la heterogeneidad de estos grupos, se seleccionaron determinados compuestos cuya importancia se debe a distintos motivos: iv ¿Fármacos que presentan una elevada resistencia a los tratamientos convencionales y por tanto una elevada persistencia en el medio ambiente, como la carbamacepina (CBZ) y el diclofenaco (DCF), cuyos efectos negativos para el medio ambiente representan un riesgo considerable. ¿Fármacos considerados menos resistentes a la degradación, cuyo abundante uso hacen que sean habitualmente detectados en distitnas masas de agua, y que también presentan efectos nocivos para el medio ambiente, como el ibuprofeno (IBU), naproxeno (NPX) y el ketoprofeno (KTP). ¿Hidrocarburos aromáticos policíclicos (PAHs), cuya elevada toxicidad, persistencia y distribución les hace representar un serio riesgo para la salud pública y el medio ambiente. Por esto son considerados contaminates prioritarios en Europa, pero a pesar de las medidas tomadas para su control siguen estando presentes en multiples ecosistemas y organismos. Para determinar la capacidad de eliminación/retención de los diferentes xenobióticos se trabajó con una instalación experimental a escala real con dos MBR independientes, ambos configurados en pre-desnitrificación y compuestos por un biorreactor anóxico, un biorreactor aireado y un tanque de membranas. Uno de los biorreactores estaba equipado con membranas planas de microfiltración fabricadas en polietileno clorado y el otro estaba equipado con membranas de fibra hueca de ultrafiltración con una trenza textil interior recubierta con polivinildenfluoruro (PVDF). Ambos MBR eran alimentados con agua residual urbana proveniente del pretratamiento de la EDAR-Sur de Granada tras el desbaste, desarenado y desengrasado. La alimentación se realizaba al reactor anóxico. Posteriormente el fango era bombeado al reactor aireado, desde el que se realizanban las purgas de fango y se alimentaba el tanque de membranas. v En el tanque de membranas existía aireación enérgica para evitar el ensuciamiento/taponamiento de las mismas y el fango concentrado era recirculado al reactor anóxico. En la instalación se midió en continuo temperatura, oxígeno disuelto y pH del fango activo. En todas las muestras de influente y efluente se analizaron sólidos en suspensión totales, sólidos en suspensión volátiles, demanda química de oxígeno (DQO), demanda biológica de oxígeno (5 días) (DBO5), las diferentes formas del nitrógeno (NH4+, NO3-, NO2-) y nitrógeno total. Y los xenobióticos se determinan en el influente, efluente, fangos activos de los distintos reactores y la purga para poder realizar un balance de materia para cada sustancia. Se realizaron también ensayos respirométricos y cultivos microbianos encaminados a determinar la toxicidad para el fango activo y la presencia de degradadores de los xenobióticos Durante la realización del presente trabajo, el HRT fue de 34 horas para el análisis de los PAHs, y de 35 horas para el resto de sustancias, mientras que el SRT fue de 12 y 25 días para los PAHs y de 37 días para los antiinflamatorios no esteroideos (IBU, NPX, KTP y DCF) , alcanzándose 40 días para la carbamacepina. En el caso de la CBZ, una elevada presencia de la misma en el agua residual mostró efectos negativos en la biomasa, pero a las pocas horas habían desaparecido y no se apreció efecto alguno en la calidad del efluente del sistema, en términos de eliminación de materia orgánica y nitrógeno. No se detectó biodegradación durante el tratamiento en el MBR y este, con un rendimiento inferior al 10 %, se mostró ineficaz en la eliminación de la CBZ. Durante el estudio con IBU, NPX, KTP y DCF se observó que la mayor parte de la eliminación de estos compuestos se realizaba en el reactor aireado. Los rendimientos para IBU, NPX y KTP fueron superiores al 95 %, similares a los registrados para la eliminación de la materia vi orgánica biodegradable. Por ello es posible afirmar que el principal mecanismo implicado en la eliminación de estos compuestos fue la biodegradación/ biotransformación. Para el DCF se observó un comportamiento similar al de la CBZ, su eliminación fue baja, incluso con rendimientos negativos en determinados periodos. Tanto la eliminación como el incremento de DCF se producían en el reactor aireado; esto indicaba la acumulación del DCF en el sistema, intensificada por la elevada recirculación y la existencia de procesos biológicos implicados en estas transformaciones. Estos rendimientos negativos también fueron observados puntualmente para la CBZ. La eficacia del sistema MBR para la eliminación de los NSAIDs analizados depende en mayor o menor medida de la capacidad de biotransformación de dichos contaminantes. Para la etapa de la investigación con los PAHs, se llevaron a cabo ensayos en biorreactores de laboratorio empleando fangos activos de un sistema MBR a escala real, y estos mostraron unos elevados rendimientos en la eliminación de fenantreno (Phen), pireno (Py) y fluoranteno (F). No se observó toxicidad durante los ensayos con PAHs, no estando estos biodisponibles. Estos resultados indicaban la importancia del mecanismo del arrastre por aire en la eliminación de estos compuestos, quedando en un segundo plano la asociación con la biomasa y cuestionando una insignificante contribución de la volatilización y la biodegradación. Se desarrolló un segundo estudio con PAHs con la intención de realizar balances de materia en un sistema MBR y poder determinar la importancia de las distintas vías de eliminación de los mismos. En el MBR a escala real, los valores para el rendimiento en la eliminación del Py y F fueron superiores al 90 %, y en el caso del Phen el rendimiento fue del 82 %. Los resultados mostraron una escasa asociación de los PAHs con la biomasa del fango activo y, aunque se habían aislado microorganismos degradadores de PAHs, destacaba la ausencia de biodegradación. Estos vii hechos revelan que el arrastre por aire es el principal mecanismo responsable de la eliminación de los PAHs en sistemas MBR. Por último, la eficiencia del proceso MBR en términos de calidad del efluente no se vio alterada ante un suceso con elevada concentración de PAHs en el influente. Por tanto, la eficacia de la tecnología MBR para la eliminación de xenobióticos presentes en aguas residuales urbanas, trabajando con elevados SRT y HRT, varía de unos compuestos a otros. Estas diferencias se deben a la distinta naturaleza química de los contaminantes que, junto con las condiciones operacionales, determinan las principales vías implicadas en la eliminación de cada compuesto. viii Abstract Lack of access to clean water and safe sanitation has been a limiting factor for development of societies and a basic element for almost all ecosystems. Proper wastewater treatment systems are essential especially in areas where limited water resources coincide with high population densities and the use of non-conventional water resources appears as a necessary option to supplement diminishing fresh water availability. Treated wastewater reuse has been increasingly used for a number of applications, including agricultural, industrial, urban and direct potable purposes. Modern society depends on a large range of organic chemicals and these may ultimately enter urban wastewater. Over the last decades, the occurrence of xenobiotic compounds in the aquatic environment has become a worldwide issue of increasing environmental concern. Xenobiotics compounds group consist of a vast array of anthropogenic as well as natural substances. The removal of some xenobiotic compounds using conventional activated sludge ix process (CASP) is often incomplete and low concentrations of these pollutants (¿g/L or ng/L) pass through the treatment plants and enter the receiving water systems. Membrane bioreactor (MBR) is an alternative membrane application in wastewater treatment. This technology combines the biological activated sludge process with solid/liquid physical separation by membrane. MBR technology merges the second and third treatment phases allowing the construction plants capable of producing directly reusable effluent. This technology is expected to enhance the removal of xenobiotics compounds produced by industrial activities and it has been selected for wastewater treatment due to this capacity. The elimination of xenobiotic compounds can occur through various mechanisms in the activated-sludge process, mainly by biodegradation, sorption or volatilization. So, their removal mechanism in MBR can defer with respect to CASP. The MBR system can operate with high SRTs and high HRTs, which may allow the development of more diverse slow-growing microbial communities capable of biodegrading specific organic compounds. A high SRT causes high biomass retention in the activated sludge, so a higher contact between biomass and pollutants is possible, increasing the adsorption of hydrophobic compounds and thereby improving the retention capacity of several pollutants. Given these characteristics, MBR systems offer a good alternative to improve the removal of pollutants such as xenobiotic compounds. The xenobiotic pollutants can be a classical persistent organic pollutant, long considered as a risk to human health and the environment due to their persistence, potential to bioaccumulation and toxicity; or they can be an emerging pollutant, these are chemicals that are not commonly monitored but have the potential to enter the environment and cause adverse ecological and human health effects. Over the last years, the occuurrence of emerging pollutants in treated wastewater has been identified as a significant environment and health concern. The present work is focused on the behaviour and removal efficiency of xenobiotic compounds during the real urban wastewater treatment by an experimental full-scale MBR working at high sludge retention time (SRT) and x high hydraulic retention time (HRT). Two of the main groups of xenobiotics were selected, pharmaceuticals products were chosen from among emerging pollutants and polycyclic aromatic hydrocarbons from among classical pollutants. Given the heterogeneity of these groups, some important compounds were selected due to different reasons: ¿Pharmaceutical pollutants which are resistant to conventional activated sludge treatment therefore they are persistent in the environment, such as carbamazepine (CBZ) and diclofenac (DCF) and their negative effects pose a risk to the environment ¿Pharmaceutical pollutants considered less resistant and more easily degradable compounds being commonly detected in different water bodies due to their abundant and widespread use, and with potential negative effects on the environment, such us ibuprofen (IBU), naproxen (NPX) and ketoprofen (KTP). ¿Polycyclic aromatic hydrocarbons (PAHs) hazardous to ecosystems and a human health risk due to their high toxicity, persistence and widespread distribution. Some of these compounds are considered priority pollutants during the last decades; however they are still commonly detected in different ecosystems and organisms. An experimental facility with two independent full-scale MBRs working in pre-denitrification configuration was used for this work. One membrane reactor was equipped with hydrophilicised micro-filtration flat-sheet membranes (0.4 ¿m nominal pore size) made of chlorine polyethylene; and the other membrane reactor was equipped with hollow fibre submerged ultrafiltration membranes (0.034 ¿m nominal pore size) made of polyvinylidenefluoride (PVDF). Both systems were composed of an anoxic bioreactor, aerobic bioreactor and membrane reactor. The facility was fed with pre-treated urban wastewater from Granada Wastewater Treatment Plant (Granada-Sur, Spain) without rubbish, sand and oils. The pre-treated wastewater was fed into xi anoxic reactor. Activated sludge of anoxic reactor was pumped to aerobic reactor which fed membrane tank. The membrane tank concentrate returned to the anoxic reactor and permeate passed to the backwashing tank, the membrane reactor was also aerated by a blower to remove solids from the membrane and to control fouling. A constant sludge purge was carried out form the aerobic reactor. Influent, effluent, purge flow, and operational parameters such as dissolved oxygen (DO), pH, temperature, and transmembrane pressure (TMP) were continuously monitored. All influent and effluent samples were analysed for total (TSS) and volatile (VSS) suspended solids, biochemical oxygen demand at five days (BOD5), chemical oxygen demand (COD), NH4+, NO3-, NO2- and total nitrogen. Activated sludge samples were analysed for TSS and VSS. The total concentrations of the selected xenobiotic compounds were determined in influent, effluent, purge, and activated sludge samples in order to determine the mass balance of each substance in the experimental MBR. Respirometric assays were made in the absence and presence of different xenobiotic compounds in order to evaluate their influence in the bacterial activity. Data were supplemented by microbiological analyses to determine the presence of culturable microorganisms capable of degrading the selected pollutants. During the experimental period with PAHs, the operational HRT was 35 h and the SRT were 12 and 25 d. While operational HRT was 34 h for the works with pharmaceutical products and the SRT was 37 d, except during the CBZ assays when SRT reached 40 d. The CBZ concentration assayed was higher than in the usual urban wastewater and negative effects were detected in the MBR bacterial community during the initial period of dosing. However, the effects were not permanent and the biomass spiked with CBZ had behaviour similar to that of the biomass without CBZ after a few hours. During and after the experimental process, CBZ did not significantly affect the efficiency of the MBR system, and the quality of the effluent xii was not affected by the dosing of CBZ in terms of COD and nitrogen removal. Biodegradation was not detected during the MBR treatment. The system showed an inefficient elimination of CBZ (less than 10%) with a high concentration in the effluent. The small percentage of CBZ removal was associated with the sludge retention and eliminated by the purge. The MBR system showed high efficiency eliminating IBU, NPX, and KTP from urban wastewater, with performance levels higher than 95%, whose main transformation occurred in the aerobic reactor with a low contribution from the anoxic reactor. The system reached a biodegradable organic matter removal higher than 99.5 % and worked with complete nitrification, also achieving an effective retention of the unbiodegradable organic matter due to recirculation. Biodegradation/biotransformation is the main mechanism involved in IBU, NPX and KTP removal by MBR. DCF removal was low with negative removal yields for several samplings. Both removal and increase transformation of DCF also occurred in the aerobic reactor, this not being observed in the anoxic one. DCF tends to accumulate in the system and to be recirculated. Thus, during the sampling in which DCF influent concentration decreases, removal yields turn negative. The increase of DCF concentration in the aerobic bioreactor also contributes to the negative removal yields. A similar behaviour was observed for CBZ. The elimination values for the NSAIDs assayed depended on the greater or lesser capacity of biotransformation on the part of the microorganisms of the activated sludge, being more significant for co-metabolisable compounds, so that the final concentrations of these compounds in the effluents will depend both on their concentration in the influent as well as their biodegradability. xiii Bench-scale experiments with experimental MBR activated sludge showed a high removal capacity for the selected PAHs. They reveal that PAHs removal is mainly due to sorption and air stripping, however the volatilization and biodegradation present a questionable insignificant contribution. Toxicity by PAHs during MBR treatment cannot be expected due to the low bio-available for the microorganisms mainly as a result of the high removal by air stripping. A second period of assays with PAHs was carried out. The fate and removal of phenanthrene (Phen), fluoranthene (F) and pyrene (Py) in urban wastewater treatment by membrane bioreactor (MBR) with low influent polycyclic aromatic hydrocarbons (PAHs) concentration were studied. All effluent samples presented concentrations of PAHs, with removal levels of 91% and 92% for F and Py respectively, while for Phen performance did not surpass 82%. Levels are lower for compounds with greater solubility in water, which are more easily carried away in the effluent. In spite of the high hydrophobicity of the tested compounds, their accumulation in the biomass was scarce and the sludge presented a low PAH concentration. The experiments reveal that PAHs removal is mainly due to air stripping, which reduces the accumulation of PAHs in the biomass and limits the establishment of microorganisms capable of biodegrading or biotransforming these compounds, most of which are released directly into the atmosphere. Biodegradation and adsorption make an insignificant contribution. Therefore, removal efficiencies of xenobiotic compounds during the real urban wastewater treatment by an experimental full-scale MBR working at high sludge retention time (SRT) and high hydraulic retention time (HRT) are diverse. Different physicochemical properties of the xenobiotic compounds and MBR operating conditions determine the main removal mechanisms. xiv Referencias Bibliográficas ¿Ahmed, F.N., Lan, C.Q. (2012). Treatment of landfill leachate using membrane bioreactors: A review. Desalination, 287, pp. 41¿54. ¿Al-Jayyousi, O.R. (2003). Greywater resuse: towards sustainable water management. Desalination, 156, pp. 181-192. ¿Al-Rifai, J. H. , Khabbaz, H., Schäfer, A. I. (2011). Removal of pharmaceutical and endocrine disrupting compounds in a water recycling process using reverse osmosis systems. 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Water Research, 35, pp. 2523-2533. ¿Camacho-Muñoz, M.D., Santos, J.L., Aparicio, I., Alonso, E. (2010). Presence of pharmaceutically active compounds in Doñana Park (Spain) main watersheds. Journal of Hazarous Materials, 177, pp. 1159 ¿ 1162. ¿Carballa, M., Omil, F., Lema, J.M. (2005). Removal of cosmetocs ingredients and pharmaceuticals in sewage primary treatment. Water Research, 39, pp. 4790-4796. ¿Carr, R.M., Blumenthal, U.J., Duncan Mara, D. (2004) Guidelines for the safe use of wastewater in agriculture: revisiting WHO guidelines. Water Science & Technology, 5 (2), pp. 31-38. ¿Carranza-Díaz, O., Schultze-Nobre, L., Moeder, M., Nivala, J., Kuschk, P., Koeser, H. (2014). Removal of selected organic micropollutants in planted and unplanted pilot-scale horizontal flow constructed wetlands under conditions of high organic load. Ecological Engineering, 71, pp. 234 ¿ 245. xviii ¿Carrara, C., Ptacek, C. J., Robertson, W. D., Blowes, D. W., Moncur, M. C., Sverko, E., Backus, S. (2008). 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The solids retention time - a suitable design parameter to evaluate the capacity of wastewater treatment plants to remove micropollutants. Water Research, 39, pp. 97¿106. ¿Clarke, B.O., Smith, S.R. (2011). Review of ¿emerging¿ organic contaminants in biosolids and assessment of international research priorities for the agricultural use of biosolids. Environmental International, 37, pp. 226 ¿ 247. ¿Cuklev, F., Fick, J., Cvijovica, M., Förlind, L., Larssona, D.G.J. (2012). Does ketoprofen or diclofenac pose the lowest risk to fish?. Journal of hazardous materials, 229-230, pp.100-106. DOI: 10.1016/j.jhazmat.2012.05.077. xix ¿Decisión 2001/2455/CE del Parlamento Europeo y del Consejo, de 20 de noviembre de 2001, por la que se aprueba la lista de sustancias prioritarias en el ámbito de la política de aguas, y por la que se modifica la Directiva 2000/60/CE. 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