Person: García Cervilla, Raúl
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First Name
Raúl
Last Name
García Cervilla
Affiliation
Universidad Complutense de Madrid
Faculty / Institute
Ciencias Químicas
Department
Ingeniería Química y de Materiales
Area
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7 results
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Item Abatement of chlorobenzenes in aqueous phase by persulfate activated by alkali enhanced by surfactant addition(Journal of Environmental Management, 2022) García Cervilla, Raúl; Santos López, Aurora; Romero, Arturo; Lorenzo Fernández, DavidSites polluted by dense non-aqueous phases (DNAPLs) constitute an environmental concern. In situ chemical oxidation (ISCO) application is limited since oxidation often occurs in the aqueous phase and contaminants are usually hydrophobic. In this work, ISCO enhanced by the surfactant addition (S–ISCO) was studied for a complex liquid mixture of chlorinated organic compounds (COCs) using persulfate (PS) activated by alkali (PSA) as oxidant and Emulse-3® as a commercial non-ionic surfactant. The reaction between E3 and PSA was investigated in the absence and presence of solubilized COCs in the following concentration ranges: COCs 1.2–50 mM, PS 84–336 mM, NaOH:PS molar ratio of 2, and surfactant concentration 1–10 g⋅L− 1. In the experiments carried out in the absence of COCs, the unproductive consumption of PS was studied. The higher the surfactant concentration, the lower the ratio PS consumed to the initial surfactant concentration due to more complex micelle structures hindering the oxidation of surfactant molecules. This hindering effect was also noticed in the oxidation of solubilized COCs. The reduction of chlorobenzenes by PSA was negligible at surfactant concentrations above 2.5 g⋅L− 1, independently of the COCs concentration solubilized. Instead, a surfactant concentration of about 1 and PS concentration of 168 mM yielded a significant decrease in the time required to abate a mass of DNAPL, compared with an ISCO process, with a bearable increase in the unproductive consumption of PSItem Remediation of the Alluvial Aquifer of the Sardas Landfill (Sabiñánigo, Huesca) by Surfactant Application(Sustainability, 2022) Guadaño, Joaquín; Gómez, Jorge; Fernández, Jesús; Lorenzo Fernández, David; Dominguez Torre, Carmen M.; Cotillas Soriano, Salvador; García Cervilla, Raúl; Santos López, AuroraSardas Landfill at Sabiñánigo Huesca is polluted with Dense Non-Aqueous Liquid Phases (DNAPLs) composed of a complex mixture of chlorinated organic compounds (COCs). This DNAPL was produced as liquid waste from lindane production being dumped decades ago in the unlined landfills close to the lindane factory. This DNAPL migrated by gravity through the subsurface and accumulated in the contact between the alluvial and marls layers (about 15 m b.g.l.). Seven injections of an aqueous emulsion of a biodegradable non-ionic surfactant (E-Mulse 3®) were carried out at the most polluted areas of the Sardas alluvial. Injections were carried out between April and November 2021 using different surfactant concentrations (6.7, 20, 25 and 50 g/L), injection volumes (0.2 to 7 m3) and injection flow rates (0.08–0.85 m3/h). Injected fluids were extracted in the same well or surrounding wells, and the time elapsed between surfactant injection and extraction varied between 24 and 72 h. A total of 22 m3 were injected into the alluvial, and more than double this injected volume was extracted. Injection and extraction points were in the contact between the marls and the alluvial layer. Extracted fluid accumulated in tanks, and phases separated. DNAPL recovered here was mobilized rather than solubilized and managed as toxic waste. The aqueous supernatant was treated in a wastewater treatment plant with physicochemical treatment (including adsorption in activated carbon) before being discharged into the environment. The transport of the injected fluids was monitored by conductivity profiles using bromide (260–538 mg·L−1) as a conservative tracer. High radial dispersion of the injected fluid was found. Surfactant losses by adsorption in the alluvial and absorption in DNAPL were noticed, and both surfactant and contamination did not escape from the capture zone. Monitoring since 2018 of the COCS in groundwater and the DNAPL presence in the contact between alluvial and marls layers showed a significant reduction of COCs in the treated zone with the surfactant injections.Item Acute Toxicity Evaluation of Lindane-Waste Contaminated Soils Treated by Surfactant-Enhanced ISCO(Molecules, 2022) Santos López, Aurora; García Cervilla, Raúl; Checa Fernández, Alicia; Domínguez, Carmen M.; Lorenzo Fernández, DavidThe discharge of lindane wastes in unlined landfills causes groundwater and soil pollution worldwide. The liquid waste generated (a mixture of 28 chlorinated organic compounds, COCs) constitutes a dense non-aqueous phase liquid (DNAPL) that is highly persistent. Although in situ chemical oxidation (ISCO) is effective for degrading organic pollutants, the low COCs solubility requires high reaction times. Simultaneous injection of surfactants and oxidants (S-ISCO) is a promising technology to solve the limitation of ISCO treatment. The current work studies the remediation of highly polluted soil (COCs = 3682 mg/kg) obtained at the Sardas landfill (Sabiñáñigo, Spain) by ISCO and S-ISCO treatments. Special attention is paid to acute soil toxicity before and after the soil treatment. Microtox®, modified Basic Solid-Phase Test (mBSPT) and adapted Organic Solvent Sample Solubilization Test (aOSSST) were used for this scope. Persulfate (PS, 210 mM) activated by alkali (NaOH, 210 mM) was used in both ISCO and S-ISCO runs. A non-ionic and biodegradable surfactant selected in previous work, Emulse®3 (E3, 5, and 10 g/L), was applied in S-ISCO experiments. Runs were performed in soil columns filled with 50 g of polluted soil, with eight pore volumes (Pvs) of the reagents injected and 96 h between successive Pv injections. The total treatment time was 32 days. The results were compared with those corresponding without surfactant (ISCO). After remediation treatments, soils were water-washed, simulating the conditions of groundwater flux in the subsoil. The treatments applied highly reduced soil toxicity (final soil toxicity equivalent to that obtained for non-contaminated soil, mBSPT) and organic extract toxicity (reduction > 95%, aOSSST). Surfactant application did not cause an increase in the toxicity of the treated soil, highlighting its suitability for full-scale applications.Item Simultaneous addition of surfactant and oxidant to remediate a polluted soil with chlorinated organic compounds: Slurry and column experiments(Journal of Environmental Chemical Engineering, 2022) García Cervilla, Raúl; Santos López, Aurora; Romero, Arturo; Lorenzo Fernández, DavidThe inadequate management of wastes associated with chlorinated organic compounds (COCs) has become a huge environmental problem. Surfactant Enhanced In-Situ Chemical Oxidation (S-ISCO) was studied as a successful technique to remediate polluted sites. This work investigated the reaction between an aqueous solution of nonionic surfactant (Emulse-3®) and an oxidant (sodium persulfate activated with NaOH) with a real polluted soil with a complex mixture of COCs from lindane liquid wastes. Two experimental setups were used. In the first one, the reactions were carried out in batch mode under slurry conditions using different surfactant concentrations (0–10 g⋅L− 1), 210 mM of persulfate and 420 mM of NaOH with an aqueous to soil ratio VL/W = 10 L⋅kg− 1. The runs were carried using a column loaded with the soil in the second experimental setup. The solution of surfactant, oxidant and activator was put in contact with soil in four pore volumes with a ratio aqueous to soil ratio VL/W = 0.2 L⋅kg− 1. Under these experimental conditions, the surfactant addition improved the reduction of COCs compared with the application carried out without surfactant, from 40.1% to values of conversion of 64.8 – 90.4%. However, an excess of surfactant hindered the COCs oxidation and increased the unproductive consumption of the oxidant, resulting in an optimal value of surfactant in the aqueous phase (1–2 g⋅L− 1). A remarkable drop in the surfactant concentration in the aqueous phase and COCs solubilized was noticed in column runs due to the surfactant adsorption.Item Partitioning of chlorinated organic compounds from dense non-aqueous phase liquids and contaminated soils from lindane production wastes to the aqueous phase(Chemosphere, 2019) Lorenzo Fernández, David; García Cervilla, Raúl; Santos López, Aurora; Romero Salvador, ArturoHexachlorocyclohexane (HCH) and mainly the g-HCH isomer, namely lindane, were extensively produced and used as pesticides. Huge amounts of wastes, solids and liquids, were disposed of in the surroundings of the production sites. The liquid residuum was a complex mixture of chlorinated organic compounds, COCs, from chlorobenzene to heptachlorocyclohexane. This Dense Non-Aqueous Phase Liquid, DNAPL, migrated by density through the subsurface to greater depths, being trapped or adsorbed into the soil in this movement posing a significant risk to the groundwater. Knowledge of the partitioning in water of COCs in DNAPL is a key issue to determine its fate in the environment. However, there are no data in literature for the partitioning and/or solubility of many of the COCs in this DNAPL, such as pentachlorocyclohexene, hexachlorocyclohexene and heptachlorocyclohexane despite them constitute about 13e30% of the mole fraction of the DNAPLs. In this work, the partitioning to water of COCs in free and those adsorbed onto soil has been studied. In addition, measured and predicted aqueous concentrations of each COC in the DNAPL mixture have been compared. To do this, the solubility of a compound that is a solid crystal when pure at P ¼ 298 K and P ¼ 1 atm has been evaluated considering the approach of sub-cooled liquid state of solid organochlorines. Samples were obtained at Sabinanigo land ~ fills and soils used had several grain sizes. Transformation in alkaline media of COCs had a positive environmental impactItem Remediation of soil contaminated by lindane wastes using alkaline activated persulfate: Kinetic model(Chemical Engineering Journal, 2020) García Cervilla, Raúl; Santos López, Aurora; Romero Salvador, Arturo; Lorenzo Fernández, DavidIn this work, remediation of a soil highly polluted with chlorinated organic compounds (COCs), including chlorobenzenes, hexachlorocyclohexane (HCH) and heptachlorocyclohexane (HeptaCH), has been carried out using persulfate (PS) activated by alkali (NaOH). The contamination was caused by wastes from lindane production. Soil samples were sieved in two fractions: F (dp < 0.25 mm) and G (2 mm < dp < 0.25 mm), and both were used to study the influence of the oxidant and activator concentrations (CPS = 100–400 mmolL−1, CNaOH =100–200molL−1) on COC abatement. The alkali causes rapid dehydrochlorination of HCHs and HeptaCHs to Trichlorobenzenes (TCBs) and Tetrachlorobenzenes (TetraCBs), respectively. A COC conversion of about 96% and 70% was obtained at 21 days in fractions G and F, respectively, when using PS and NaOH concentrations of 400 mmolL−1. The discriminated kinetic model reveals that the oxidation reaction takes place in both the soil and aqueous phases. This explains in detail the TCB and TetraCB concentration change seen in both phases with the reaction time, at the oxidant and activator concentration range studied, for the two soil particle sizes and contamination levels used. Reaction order for NaOH concentration was zero if pH was above 12. The reaction order for PS was 1.0 for the oxidation rate in the aqueous phase and lower than 1.0 for the oxidation rate in the soil phase, which is lower in the soil fraction with smaller particles. Moreover, while equilibrium between phases was not achieved, the model takes into account the mass transfer of COCs from the soil to the aqueous phaseItem Compatibility of nonionic and anionic surfactants with persulfate activated by alkali in the abatement of chlorinated organic compounds in aqueous phase(Science of The Total Environment, 2020) García Cervilla, Raúl; Santos López, Aurora; Romero Salvador, Arturo; Lorenzo Fernández, DavidSurfactant Enhanced In-Situ Chemical Oxidation (S-ISCO) is an emerging technology in the remediation of sites with residual Dense Non-Aqueous Phase Liquids (DNAPLs), a ubiquitous problem in the environment and a challenge to solve. In this work, three nonionic surfactants: E-Mulse3® (E3), Tween80 (T80), and a mixture of Tween80-Span80 (TS80), and an anionic surfactant: sodium dodecyl sulfate (SDS), combined with persulfate activated by alkali (PSA) as oxidant have been investigated to remove the DNAPL generated as liquid waste in lindane production, which is composed of 28 chlorinated organic compounds (COCs). Because the compatibility between surfactants and oxidants is a key aspect in the S-ISCO effectiveness the unproductive consumption of PS by surfactants was investigated in batch (up to 864 h) varying the initial concentration of PS (84–42 mmol·L−1 ) and surfactants (0–12 g·L−1 ) and the NaOH:PS molar ratio (1 and 2). The solubilization capacity of a partially oxidized surfactant was analyzed by estimating its Equivalent Surfactant Capacity, ESC, (as mmolCOCs dissolved gsurf −1) and comparing it to the expected value for an unoxidized surfactant, ESCo. Finally, the abatement of DNAPL with simultaneous addition of surfactant and PSA was studied. At the conditions used, a negligible unproductive consumption of PS was found by SDS; meanwhile, PS consumption at 360 h ranged between 70 and 80% using the nonionic surfactants. The highest ratios of ESC/ESCo were found with SDS and E3 and these surfactants were chosen for the S-ISCO treatment. When oxidant and surfactant were simultaneously applied for DNAPL abatement the COC conversion was more than three times higher with E3 (0.6 at 360 h) than SDS. Moreover, it was obtained that the time needed for the removal of a mass of DNAPL by PSA in the absence of surfactants was notably higher than the time required when a suitable surfactant was added