Browsing by Author "Destaillats, Hugo"

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    Effect of different gases on the sonochemical Cr(VI) reduction in the presence of citric acid
    (2020-12-01) Meichtry, Jorge Martín; Cancelada, Lucía; Destaillats, Hugo; Litter, Marta Irene
    The sonochemical (850 kHz) Cr(VI) reduction (0.30 mM, pH 2) in the presence of citric acid (Cit, 2 mM) was analyzed under different working atmospheres: reactor open to air without sparging (ROAWS), and Ar, O2, air and N2 sparging. Hydrogen peroxide formation in pure water at pH 2 and KI dosimetry were also measured. Zero-order kinetics was observed in all cases. A complete Cr(VI) reduction after 180 min insonation was obtained with the ROAWS and under Ar, while a lower Cr(VI) reduction efficiency was achieved under the other conditions. The Cr(VI) reduction and H2O2 formation rates followed the order ROAWS ?° Ar > air ?° O2 >> N2, while for KI dosimetry the order was ROAWS >> O2 ?° air > Ar >> N2. This indicates that H2O2 formation rate is a better measure of the system reactivity for Cr(VI) reduction. For air, O2 and N2, once the sparging was stopped, Cr(VI) reduction rate increased up to approximately the same value obtained for the ROAWS, suggesting that the sparging decreased the generation of reactive species and, thus, the Cr(VI) reduction rate. Nitrate production was measured at low concentrations (micromolar range) in the ROAWS, air and N2 systems. Formic and acetic acids were detected as Cit degradation products. Reaction mechanisms were proposed. It can be concluded that the best conditions for Cr(VI) removal are with the ROAWS because of a higher Cr(VI) reduction rate, no atmosphere control is required, and it is a less expensive system.
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    Synergetic combination of nano zero-valent iron, ultrasound and carboxylic acids for the removal of aqueous Cr(VI)
    (2023-06-08) Cancelada, Lucía; Meichtry, Jorge Martín; Destaillats, Hugo; Litter, Marta Irene
    Cr(VI) is a priority pollutant present in wastewater of several industrial processes such as electroplating and leather tanning; it can be also naturally present in groundwater. The usual treatment of Cr(VI) involves its reduction to Cr(III), a far less toxic and mobile species, which can be precipitated from the solution at circumneutral pH values [1]. However, conventional Cr(VI) chemical reductants, such as Fe(II) salts, require large Fe:Cr molar ratios to be efficient, generating the disposal of large amounts of dangerous sludge. Thus, more efficient Cr(VI) reduction treatments are required. In this work, the efficiency of commercial zero-valent iron nanoparticles (nZVI), ultrasound (US), and carboxylic acids (CAs) for Cr(VI) reduction was evaluated. The CAs used were citric acid (Cit) or ethylenediaminetetraacetic acid (EDTA). The experiments were performed with 200 mL of a 0.3 mM Cr(VI) solution at pH 3 and under air bubbling (0.5 L min-1) at 30 °C for 180 min in an ultrasonic reactor (850 kHz, total power input 35 W L-1). NSTAR (Nanoiron®) was used as nZVI, with a 3:1 Fe:Cr molar ratio (the optimal ratio as determined before for N25 nZVI [2]), Cit (0 or 2 mM) or EDTA (0 or 1 mM). In the absence of Cit or EDTA (nZVI alone or nZVI + US), or with Cit or EDTA alone (neither nZVI nor US), Cr(VI) reduction was negligible (≤ 5% of the initial [Cr(VI)]). US + Cit showed a reduction of 49% of the initial [Cr(VI)], while US + EDTA showed a 32% of reduction. On the other hand, nZVI + US + Cit yielded an 88% of Cr(VI) reduction, which was 60% with nZVI + US + EDTA. This indicates a clear synergy within the ternary system (nZVI + US + CAs). In all cases, the evolution of Cr(VI) could be fitted to a zero-order kinetic model , with R2 values higher than 0.94. NSTAR nZVI particles are composed of a zerovalent Fe core surrounded by a protective shield of iron oxides that inhibits Cr(VI) reduction; thus, only the combination of US and CAs can remove this protective shield and enhance Cr(VI) reduction, being Cit more efficient than EDTA. This was reinforced by the monitoring of the evolution of the total Fe concentration in solution, with final values of 0.076, 0.26, and 0.18 mM for the systems nZVI + US, nZVI + US + Cit and nZVI + US + EDTA, respectively, indicating that Cit and EDTA promote the formation of soluble Fe complexes. Besides, in the previous experiments of US without nZVI, Cit also proved to be a better donor than EDTA, probably because it can stabilize to a higher extent intermediate peroxo-Cr(V) compounds [1]. Summarizing, there is a synergy for Cr(VI) reduction in the ternary system nZVI + US + CAs, being Cit more efficient than EDTA.