Research Outputs

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Application of high silica zeolite ZSM-5 in a hybrid treatment process based on sequential adsorption and ozonation for VOCs elimination

2016, Dr. Valdes-Morales, Hector, Zaitan, Hicham, Manero, Marie

In this study, a hydrophobic synthetic zeolite, namely ZSM-5 is chosen as an adsorbent/ catalyst for toluene removal. Experimental results showed that toluene adsorption onto ZSM-5 was favourable, following a Langmuir adsorption isotherm model. ZSM-5 zeolite was regenerated using gaseous ozone at low temperature. Adsorbed toluene was oxidised, releasing mainly CO2 and H2O. Traces of oxidation by-products such as acetic acid and acetaldehyde were formed and remained adsorbed after the oxidativate regeneration with ozone. After four successive cycles of adsorption/ozonation, the adsorption efficiency was not affected (92%–99%). These results showed that volatile organic compound (VOC) removal by adsorption onto ZSM-5 zeolite followed by ozone regeneration could be used as a promising hybrid process for the control of VOC emissions in terms of efficiency.

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Removal of benzothiazole from contaminated waters by ozonation: The role of direct and indirect ozone reactions

2016, Dr. Valdes-Morales, Hector, Zaror, Claudio, Jekel, Martin

Benzothiazoles are emerging chemical pollutants mainly coming from leather, paper and rubber industries; due to their use as: herbicides, corrosion inhibitors, anti-freezers, and vulcanisation accelerators. This article presents experimental data on ozone treatment of benzothiazole contaminated waters. The effect of the initial concentration of benzothiazole, ozone dosage, temperature (10-30 °C), and pH (2-9), on ozonation removal rate were assessed at bench scale. Experimental results show that reaction between ozone and benzothiazole could be approximated to a second-order kinetic law. Kinetic parameters for direct and indirect ozone reactions are estimated and temperature dependence of rate parameters is evaluated. Moreover, an initial degradation pathway of benzothiazole ozonation is proposed.

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New insight of the influence of acidic surface sites of zeolite on the ability to remove gaseous ozone using operando DRIFTS studies

2020, Valdes-Morales, Hector, Ulloa, Francisco J., Solar, Víctor A., Cepeda, Manuel S., Azzolina-Jury, Federico, Thibault-Starzyk, Frédéric

Recently, natural zeolites have started to be used as alternative materials for ozone abatement from working environments. In this study, a surface response methodology based on a D-Optimal design is applied to develop a transition-metal-modified natural zeolite that increases ozone removal efficiency. Ozone adsorption and/or decomposition onto natural and cobalt modified natural zeolite were studied by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Results evidenced that ozone is adsorbed and decomposed at strong Lewis acidic sites, whereas ozone adsorption products interact with surface OH groups. Additionally, DRIFTS studies indicate that nitrous species are adsorbed at acidic sites, reducing the capacity to decompose ozone when ozone is generated from air.

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Gaseous ozone decomposition over high silica zeolitic frameworks

2018, Brodu, Nicolas, Manero, Marie-Hélène, Andriantsiferana, Caroline, Pic, Jean-Stéphane, Valdes-Morales, Hector

For several decades, it has been known that ozone emissions are harmful to humans, plants, and animals. Heterogeneous catalytic decomposition is an efficient process for removing ozone from air. This study examines the effect of the zeolite's framework and pore width on efficiency for decomposing gaseous ozone. Four highly hydrophobic zeolites are used: a large cavity zeolite (Faujasite/H‐FAU), a medium pore zeolite with parallel channel (Mordenite/H‐MOR), and two medium pore zeolites with interconnected channels (H‐ZSM‐5/H‐MFI and Na‐ZSM‐5/Na‐MFI). Experiments were conducted in fixed‐bed flow reactors loaded with zeolite at ambient conditions (20 °C and 101 kPa). Zeolite surfaces were analyzed during the experiments in order to understand the influence of physical and chemical surface properties on the ozone decomposition mechanism. A higher amount of ozone is eliminated using H‐MOR, compared with the zeolite samples H‐FAU, H‐MFI, and Na‐MFI. Pore width and micropore framework size distribution (channel and cages) appear to be key factors. A narrow channel or cage, slightly larger than the ozone molecule size, seems to promote ozone interactions with Lewis acid sites. Fourier transform infrared spectroscopy shows that Lewis acid sites (LAS), located on the walls of zeolite pores, decompose ozone. This leads to the formation of atomic oxygen species that could react with another ozone molecule to form dioxygen. Hence, LAS are regenerated, ready to decompose another ozone molecule once more.