Person:
García Rodríguez, Juan

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First Name
Juan
Last Name
García Rodríguez
URI
https://hdl.handle.net/20.500.14352/76093
Affiliation
Universidad Complutense de Madrid
Faculty / Institute
Ciencias Químicas
Department
Ingeniería Química y de Materiales
Area
Ingeniería Química
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    Efficient removal of antibiotic ciprofloxacin by catalytic wet air oxidation using sewage sludge-based catalysts: degradation mechanism by DFT studies
    (Journal of Environmental Chemical Engineering, 2023) Gutiérrez Sánchez, Pablo; Álvarez Torrellas, Silvia; Larriba Martínez, Marcos; Gil, María Victoria; Garrido Zoido, Juan Manuel; García Rodríguez, Juan
    In this work, the sewage sludge-derived activated carbon (SAC) loaded with iron nanoparticles (FeSAC) showed a highly effective catalytic activity in the degradation of the antibiotic ciprofloxacin by the CWAO reaction. The properties of FeSAC catalyst were studied by using N2 adsorption-desorption measurements at 77 K, scanning electron microscopy, X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy and thermogravimetric analysis. The CWAO reaction was evaluated at different temperatures (120–140 ºC), total pressure (10–30 bar) and catalyst doses (0.1–0.7 g/L) in a batch reactor. In this regard, temperature and catalyst dosage showed a significant impact on the removal of the tested antibiotic. By using a catalyst dose of 0.7 g/L, ciprofloxacin degradation and CO2 selectivity were higher than 99 % and 60 %, respectively, and were achieved within two hours at 140 °C and 20 bar. The loss of the active phase (Fe) of the catalyst in the reaction medium was measured, obtaining negligible values (less than 24 ppb). This catalyst showed high stability under the tested reaction conditions. In addition, a potential equation was proposed to correctly describe the evolution of ciprofloxacin degradation. The calculated activation energy of the CWAO process was 53.8 kJ/mol. Additionally, Density Functional Theory (DFT) calculations were performed to illustrate the degradation mechanism of ciprofloxacin, where the electronic energies indicated the compounds that are most difficult to degrade by CWAO. Finally, a proof of concept using an environmentally-relevant matrix was carried out, verifying the technical feasibility of the synthesized catalyst for its application with more complex matrices, consecutive reaction cycles and at a low treatment cost
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    Insights of emerging contaminants removal in real water matrices by CWPO using a magnetic catalyst
    (Journal of Environmental Chemical Engineering, 2021) Huacallo Aguilar, Ysabel; Álvarez Torrellas, Silvia; Gil, Maria Victoria; Larriba Martínez, Marcos; García Rodríguez, Juan
    The study was focused on the application of catalytic wet peroxide oxidation (CWPO) with a synthesized magnetic catalyst (Fe3O4/MWCNTs) for the treatment of real water matrices spiked with pharmaceutical compounds. CWPO was carried out by modifying the initial pH of surface water (SW), wastewater treatment plant (WWTP) effluent, brewery wastewater (BW) and hospital wastewater (HW), and the effect of the addition of the emerging pollutants naproxen (NAP) and diclofenac (DCF). From the experimental results, pH and concentration of NAP and DCF in CWPO were crucial factors in the successful pollutants removal from water matrices. The lab-prepared catalyst showed high removal rates of NAP and DCF from different water matrices spiked with the NAP-DCF mixture at pH 5.0. The highest average removal rate of TOC (75%), NAP (66%), DCF (76%), TN (39%) and aromaticity (68.39%) was obtained for SW matrix using 1.0 g L−1 of catalyst, pH ≈ 5.0, 5 mM of H2O2 and 60 °C. The mineralization decreased with the increase of the initial TOC concentration of the tested matrix. By CWPO tests of the real water matrices it was demonstrated that DCF removal was higher than NAP. From the recyclability tests, the catalyst demonstrated high activity and stability along three consecutive CWPO cycles of 8 h each one. The pseudo-second order model well-described the degradation of NAP and DCF. Finally, aromaticity and toxicity of the effluents were greatly reduced after CWPO treatment. This work demonstrated that CWPO with the magnetic catalyst is an efficient method to remove DCF-NAP mixtures from real aqueous matrices