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104. Near UV‐Irradiation of CuOx‐Impregnated TiO2 Providing Active Species for H2 Production Through Methanol Photoreforming

Author

Vitiello, Giuseppe, primary, Clarizia, Laura, additional, Abdelraheem, Wael, additional, Esposito, Serena, additional, Bonelli, Barbara, additional, Ditaranto, Nicoletta, additional, Vergara, Alessandro, additional, Nadagouda, Mallikarjuna, additional, Dionysiou, Dionysios D., additional, Andreozzi, Roberto, additional, Luciani, Giuseppina, additional, and Marotta, Raffaele, additional

Published
2019
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105. Simulated Moon Agglutinates Obtained from Zeolite Precursor by Means of a Low-Cost and Scalable Synthesis Method

Author

Freyria, Francesca S., primary, Marocco, Antonello, additional, Esposito, Serena, additional, Bonelli, Barbara, additional, Barrera, Gabriele, additional, Tiberto, Paola, additional, Allia, Paolo, additional, Oudayer, Pauline, additional, Roggero, Aurélien, additional, Matéo-Vélez, Jean-Charles, additional, Dantras, Eric, additional, and Pansini, Michele, additional

Published
2019
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108. Magnetic Properties of Nanocomposites

Author

Barrera, Gabriele, primary, Tiberto, Paola, additional, Allia, Paolo, additional, Bonelli, Barbara, additional, Esposito, Serena, additional, Marocco, Antonello, additional, Pansini, Michele, additional, and Leterrier, Yves, additional

Published
2019
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110. Ru/RuO2@Nb2O5-SiO2 Nanomaterials for Hydrogenation of Levulinic Acid in the Aqueous-phase

Author

MINIERI, LUCIANA, ESPOSITO, SERENA, RUSSO, VINCENZO, DI SERIO, MARTINO, ARONNE, ANTONIO, SILVESTRI, BRIGIDA, Bonelli, Barbara, Luciana Minieri , Serena Esposito, Vincenzo Russo, Barbara Bonelli, Martino Di Serio , Antonio Aronne, Brigida Silvestri, Minieri, Luciana, Esposito, Serena, Russo, Vincenzo, Bonelli, Barbara, DI SERIO, Martino, Aronne, Antonio, and Silvestri, Brigida

Published
2016

111. Nanomaterials for the Abatement of Pharmaceuticals and Personal Care Products from Wastewater

Author

Massachusetts Institute of Technology. Department of Chemistry, Freyria, Francesca S, Geobaldo, Francesco, Bonelli, Barbara, Massachusetts Institute of Technology. Department of Chemistry, Freyria, Francesca S, Geobaldo, Francesco, and Bonelli, Barbara

Abstract

In this short-review, the most common types of both pharmaceutical and personal care products (PPCP, a class of “emerging pollutants”) are considered, as well as some of the most frequent methods for their removal that envisage the use of nanomaterials. The nanomaterials used in conservative methods (namely, reverse osmosis, nanofiltration and adsorption) are basically nanoporous solids. Non-conservative methods, which include photocatalysis and Fenton reaction, are currently considered more promising than conservative ones, as the former allow the (at least) partial degradation of the original molecules into more biodegradable by-products, which can be further abated by subsequent biological treatments, whereas the former are not efficient for the removal of small quantities of pollutants and have to be regenerated. Keywords: emerging pollutants; PPCPs; photocatalysis; nanomaterials, Fondazione Cariplo (Grant 2015–0186)

Published
2018

112. Development of Unconventional Photocatalytic Reactors and Processes for the Abatement of Harmful N-containing Pollutants

Author

Rossetti, Ilenia, Compagnoni, Matteo, Ramis, Gianguido, Freyria, Francesca, Armandi, Marco, and Bonelli, Barbara

Subjects
lcsh:Computer engineering. Computer hardware, lcsh:TP155-156, Chemical Engineering (all), lcsh:TK7885-7895, lcsh:Chemical engineering
Abstract

In the present work, innovative photocatalytic processes were developed for the abatement of harmful N- containing compounds, focusing on selectivity towards innocuous N2, to be applied for the treatment of waste waters to meet legislative specifications. The photocatalytic performance of the samples has been checked for the photoreduction of nitrate ions, the photooxidation of ammonia and of organic N-containing compounds. Catalytic performance was correlated with the properties of the nanomaterials. Two innovative semi-batch photoreactors were specifically designed and optimized for this application. Different photocatalysts have been compared. TiO2 has been prepared in nanosized form by using an innovative flame pyrolysis (FP) approach, able to synthesise in one step single or mixed oxide nanoparticles, characterized by homogeneous particle size and good phase purity. In some cases Pd has been added to TiO2 by post synthesis impregnation. The role of the metal nanoparticles was the enhancement of the lifetime of the photoproduced charges by electron trapping. The same materials formulations have been prepared starting from commercial nanostructured TiO2 supports for comparison purposes. The addition of Pd revealed the key to improve both the conversion and the selectivity to N2. The FP prepared materials were in general more active than the commercial TiO2 P25 sample.

Published
2017

114. How Many Chemical Elements are there in the Universe? A (not so) Bohring Question

Author

Garrone, Edoardo, Areán, C. O., and Bonelli, Barbara

Subjects
general chemistry, Ununseptium, island of stability, atomic number, Bohr atomic model, periodic table, hydrogenoid atom, Bohr atomic model, general chemistry, base chemistry course, periodic table, hydrogenoid atom, speed of light, Ununseptium, island of stability, atomic number, speed of light, base chemistry course
Published
2017

115. Mesoporous Titania : Synthesis, Properties and Comparison With Non-Porous Titania

Author

Bonelli, Barbara

Subjects
Science / Chemistry / Inorganic
Abstract

Some relevant physico-chemical and photocatalytic properties of ordered mesoporous TiO2 as obtained by template-assisted synthesis methods are reported. After a review of the crucial aspects related to different synthesis procedures reported by the literature, the focus is pointed on the (often) superior physico-chemical properties of ordered mesoporous TiO2 with respect to (commercial) bulk TiO2. Those are essentially higher specific surface area and ordered mesoporosity; possibility to control the formation of different crystalline phases by varying the synthesis conditions and possibility to obtain films, nanoparticles with different morphologies and/or materials with hierarchical porosity. Although mesoporous TiO2 is extensively studied for many applications in the fields of photocatalysis, energy and biomedicine, this chapter focuses on the use of mesoporous TiO2 in environmental photocatalysis, by putting in evidence how the physico-chemical properties of the material may affect its photocatalytic behaviour and how mesoporous TiO2 behaves in comparison with commercial TiO2 samples.

Published
2017

116. Effects of the Brookite Phase on the Properties of Different Nanostructured TiO2 Phases Photocatalytically Active Towards the Degradation of N‐Phenylurea.

Author

Freyria, Francesca S., Blangetti, Nicola, Esposito, Serena, Nasi, Roberto, Armandi, Marco, Annelio, Vincenzo, and Bonelli, Barbara

Subjects
PORE size distribution, X-ray powder diffraction, RIETVELD refinement, TRANSMISSION electron microscopy, ISOELECTRIC point, NANOSILICON
Abstract

Different sol‐gel synthesis methods were used to obtain four nanostructured mesoporous TiO2 samples for an efficient photocatalytic degradation of the emerging contaminant N‐phenylurea under either simulated solar light (1 Sun) or UV light. Particularly, two TiO2 samples were obtained by means of as many template‐assisted syntheses, whereas other two TiO2 samples were obtained by a greener template‐free procedure, implying acidic conditions and, then, calcination at either 200 °C or 600 °C. In one case, anatase was obtained, whereas in the other three cases mixed crystalline phases were obtained. The four TiO2 samples were characterized by X‐ray powder diffraction (followed by Rietveld analysis); Transmission Electron Microscopy; N2 adsorption/desorption at −196 °C; Diffuse Reflectance UV/Vis spectroscopy and ζ‐potential measurements. A commercial TiO2 powder (i. e., Degussa P25) was used for comparison. Differences among the synthesized samples were observed not only in their quantitative phase composition, but also in their nanoparticles morphology (shape and size), specific surface area, pore size distribution and pHIEP (pH at isoelectric point), whereas the samples band‐gap did not vary sizably. The samples showed different photocatalytic behavior in terms of N‐phenylurea degradation, which are ascribed to their different physico‐chemical properties and, especially, to their phase composition, stemming from the different synthesis conditions. [ABSTRACT FROM AUTHOR]

Published
2020
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123. Molecular water on exposed A[l.sup.3+] cations is a source of acidity in silicoaluminas

Author

Garrone, Edoardo, Onida, Barbara, Bonelli, Barbara, Busco, Claudia, and Ugliengo, Piero

Subjects
Aluminum silicates -- Chemical properties, Water chemistry -- Research, Chemicals, plastics and rubber industries
Abstract

A study using infrared spectroscopy and ab initio calculations provided evidence about the remarkable acidic nature of molecular water adsorbed at the surface of mesoporous MCM-41 silicoaluminas (MSA) with a ratio of Si/Al = 25. OH stretching and HOH bending modes of water adsorbed on coordinatively unsaturated Al ions at the surface of mesoporous version of silicoaluminas were detected for the first time using CO as a probe.

Published
2006

131. Preparation and Characterization of Magnetic and Porous Metal-Ceramic Nanocomposites from a Zeolite Precursor and Their Application for DNA Separation

Author

Pansini, Michele, primary, Dell'agli, Gianfranco, additional, Marocco, Antonello, additional, Netti, Paolo Antonio, additional, Battista, Edmondo, additional, Lettera, Vincenzo, additional, Vergara, Paola, additional, Allia, Paolo, additional, Bonelli, Barbara, additional, Tiberto, Paola, additional, Barrera, Gabriele, additional, Alberto, Gabriele, additional, Martra, Gianmario, additional, Arletti, Rossella, additional, and Esposito, Serena, additional

Published
2017
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132. SO2deactivation mechanism of NO oxidation and regeneration of the LaCoO3perovskiteElectronic supplementary information (ESI) available. See DOI: 10.1039/c9cy02478f

Author

Martinovic, Ferenc, Tran, Quang Nguyen, Deorsola, Fabio Alessandro, Bensaid, Samir, Palkovits, Regina, Paulus, Werner, Bonelli, Barbara, Di Renzo, Francesco, and Pirone, Raffaele

Abstract

The deactivation mechanism and methods to cope with the poisoning by SO2of LaCoO3perovskite-based NO oxidation catalysts were investigated. The LaCoO3perovskite was synthesized by a sol–gel method and the fresh, sulphate-deactivated and regenerated catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, H2-and soot-temperature programmed reduction, temperature programmed desorption and diffuse reflectance infrared Fourier transform spectroscopy. The SO2poisoning strongly affected the NO oxidation activity. It was demonstrated that the deactivation mechanism proceeds in two stages: initially the active sites with a basic character are blocked by SO3and subsequently the lanthanum sulphate salts grow progressively on the surface and cobalt is unaffected. Above 500 °C, the surface bound sulphates become mobile and migrate into the bulk of the catalyst. Several prevention and regeneration methods were proposed and tested. By mixing the catalyst with Ca(OH)2as an adsorbent nearly 50% of the original activity was retained. Regeneration by diesel soot was presented here for the first time, where the blocking oxygen can spill over to the soot oxidizing it and releasing the bound sulphur as SO2and CO2. Furthermore, a facile regeneration method was explored by washing the deactivated catalyst to dissolve the small amounts of sulphates on the surface.

Published
2020
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133. Near UV‐Irradiation of CuOx‐Impregnated TiO2 Providing Active Species for H2 Production Through Methanol Photoreforming.

Author

Vitiello, Giuseppe, Clarizia, Laura, Abdelraheem, Wael, Esposito, Serena, Bonelli, Barbara, Ditaranto, Nicoletta, Vergara, Alessandro, Nadagouda, Mallikarjuna, Dionysiou, Dionysios D., Andreozzi, Roberto, Luciani, Giuseppina, and Marotta, Raffaele

Subjects
ELECTRON paramagnetic resonance spectroscopy, ELECTRON microscope techniques, METHANOL production, COPPER oxidation, TRANSMISSION electron microscopes
Abstract

Copper doped‐TiO2 (P25) nanomaterials have been intensively studied as promising catalysts for H2 production by photo‐reforming of selected organic compounds. However, the role of copper oxidation states on the improvement of photocatalytic activity is still debated. In this work, CuOx‐impregnated P25‐TiO2 catalysts were used for photocatalytic production of hydrogen from methanol. Copper species/oxidation states both in the as‐prepared catalysts and after the photocatalytic process were investigated. To this purpose, H2 production rates were correlated to physico‐chemical properties of the samples, both before and after photocatalytic process, by means of Raman, X‐Ray Diffraction, Electron Paramagnetic Resonance spectroscopy, X‐Ray Photoelectron Spectroscopy, Temperature‐Programmed Reduction and High Resolution Transmission Electron Microscope techniques. Results revealed the presence of both Cu2O and CuO deposits on the samples surface after calcination. Notably, under near‐UV irradiation, the fraction of highly dispersed CuO particles undergo a partial dissolution process, followed by reduction to metallic copper Cu(s) by photogenerated electrons, boosting H2 production rate. Our findings indicate that both Cu2O and Cu(s) act as co‐catalysts for H2 generation, yet by different mechanisms. Overall this study, provides the basis to enhance catalytic performance of red‐ox active systems through UV‐irradiation approach. [ABSTRACT FROM AUTHOR]

Published
2019
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134. IR evidence that secondary interactions may hamper H-bonding at protonic sites in zeolites

Author

Onida, Barbara, Bonelli, Barbara, Borello, Luisa, Fiorilli, Sonia, Geobaldo, Francesco, and Garrone, Edoardo

Subjects
Molecules -- Spectra, Hydrogen bonding -- Research, Zeolites -- Spectra, Chemicals, plastics and rubber industries
Abstract

When a molecule, engaged in H-bonding with an acidic proton in zeolites, is large enough to interact with the surrounding walls, the IR spectroscopic measure of the acidity is affected, but information may be gained on the geometry of the site. Examples concerning MCM-22, ZSM-5, SAPO-40, and Theta-1 are deiscussed.

Published
2002

135. Salicylic Acid-Modified Sm-TiO2for Photoluminescence and Photocatalysis under Real Sunlight: Synergistic Effects between Ligand-to-Metal Charge Transfer (LMCT) and Sm3+Dopant

Author

Lakhdar, Rostom, Freyria, Francesca S., Mousdis, George A, Bonelli, Barbara, and Elghniji, Kais

Abstract

A salicylic-acid (SA)-modified samarium-doped TiO2complex (Sm-TiO2/SA) was synthesized via a sol–gel method followed by impregnation. A Raman Fourier transform IR and X-ray photoelectron spectroscopic study showed that SA (as an electron donor) forms a surface complex on the Sm-TiO2surface through its phenolic/carboxylic functional groups. In the Sm-TiO2/SA complex, a ligand-to-metal charge transfer (LMCT) is active, inducing a marked red-shift in the absorption spectrum of TiO2, which extends to 550–600 nm. The synergetic effect between the LMCT process and the luminescent properties of the lanthanide ions (Sm3+) is discussed and supported by the photoluminescence spectra. Further photocatalytic experiments (under sunlight) and the study of the effect of different scavengers show the presence of competitive reactions between de-ethylation and cleavage of Rhodamine B (RhB) during its degradation. With the Sm-TiO2/SA complexes, the superoxide radical ion (O2•–) is the main active species responsible for the N-de-ethylation pathway under sunlight irradiation. The cleavage of RhB by the hydroxyl radical (•OH) appears, instead, to dominate with the Sm-TiO2photocatalysts.

Published
2024
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136. Al/Fe isomorphic substitution versus Fe[subscript2]O[subscript 3] clusters formation in Fe-doped aluminosilicate nanotubes (imogolite)

Author

Massachusetts Institute of Technology. Department of Chemistry, Freyria, Francesca Stefania, Shafia, Ehsan, Esposito, Serena, Manzoli, Maela, Chiesa, Mario, Tiberto, Paola, Barrera, Gabriele, Menard, Gabriel, Allia, Paolo, Garrone, Edoardo, Bonelli, Barbara, Massachusetts Institute of Technology. Department of Chemistry, Freyria, Francesca Stefania, Shafia, Ehsan, Esposito, Serena, Manzoli, Maela, Chiesa, Mario, Tiberto, Paola, Barrera, Gabriele, Menard, Gabriel, Allia, Paolo, Garrone, Edoardo, and Bonelli, Barbara

Abstract

Textural, magnetic and spectroscopic properties are reported of Fe-doped aluminosilicate nanotubes (NTs) of the imogolite type, IMO, with nominal composition (OH)[subscript 3]Al[subscript 2−x]Fe[subscript x]O[subscript 3]SiOH (x = 0, 0.025, 0.050). Samples were obtained by either direct synthesis (Fe-0.025-IMO, Fe-0.050-IMO) or post-synthesis loading (Fe-L-IMO). The Fe content was either 1.4 wt% (both Fe-0.050-IMO and Fe-L-IMO) or 0.7 wt% (Fe-0.025-IMO). Textural properties were characterized by High-Resolution Transmission Electron Microscopy, X-ray diffraction and N[subscript 2] adsorption/desorption isotherms at 77 K. The presence of different iron species was studied by magnetic moment measurements and three spectroscopies: Mössbauer, UV–Vis and electron paramagnetic resonance, respectively. Fe[superscript 3+]/Al[superscript 3+] isomorphic substitution (IS) at octahedral sites at the external surface of NTs is the main process occurring by direct synthesis at low Fe loadings, giving rise to the formation of isolated high-spin Fe[superscript 3+] sites. Higher loadings give rise, besides IS, to the formation of Fe[subscript 2]O[subscript 3] clusters. IS occurs up to a limit of Al/Fe atomic ratio of ca. 60 (corresponding to x = 0.032). A fraction of the magnetism related to NCs is pinned by the surface anisotropy; also, clusters are magnetically interacting with each other. Post-synthesis loading leads to a system rather close to that obtained by direct synthesis, involving both IS and cluster formations. Slightly larger clusters than with direct synthesis samples, however, are formed. The occurrence of IS indicates a facile cleavage/sealing of Al–O–Al bonds: this opens the possibility to exchange Al[superscript 3+] ions in pre-formed IMO NTs, a much simpler procedure compared with direct synthesis.

Published
2016

137. Hydrogen storage via physisorption: the combined role of adsorption enthalpy and entropy

Author

AREAN, Carlos Otero and BONELLI, Barbara

Subjects
Adsorption thermodynamics, enthalpy-entropy correlation, hydrogen physisorption, hydrogen storage
Abstract

Materials capable of cost-effective on-board hydrogen storage and delivery are currently being sought worldwide as a means to facilitate a hydrogen-based energy transition in the transportation sector. Among the solutions proposed, hydrogen storage by physisorption on porous solids constitutes a main avenue of research, and for intelligent design of such materials a detailed knowledge of gas adsorption thermodynamics is of the utmost importance. Analysis of the available data for hydrogen adsorption on alkali and alkaline-earth cation exchanged zeolites clearly shows that standard adsorption enthalpy (D H0) and entropy (D S0) are correlated, in the sense that larger D S0 values correspond to larger D H0 values. It was also shown that, referring to absolute values, the relative rate at which adsorption entropy changes decreases gradually as adsorption enthalpy increases thus resulting in a non-linear correlation between D H0 and D S0. These results are discussed and corresponding implications for hydrogen storage via physisorption are highlighted.

Published
2014

138. Imogolite: An Aluminosilicate Nanotube Endowed with Low Cytotoxicity and Genotoxicity

Author

Bianca Maria Rotoli, Patrizia, Guidi, Bonelli, Barbara, Margherita, Bernardeschi, Bianchi, Massimiliano G., Serena, Esposito, Giada, Frenzilli, Paolo, Lucchesi, Marco, Nigro, Vittoria, Scarcelli, Maura, Tomatis, Pier Paolo Zanello, Bice, Fubini, Ovidio, Bussolati, Enrico, Bergamaschi, and Esposito, Serena

Subjects
imogolite, genotoxicity, citotoxicity, Formates, Free Radicals, Cell Survival, single walled nanotube, Nitric Oxide, Toxicology, medicine.disease_cause, Cell Line, Mice, chemistry.chemical_compound, Cell Line, Tumor, medicine, aluminum silicate, Animals, Humans, Organic chemistry, aluminum silicate, DNA, inducible nitric oxide synthase, multi walled nanotube, nitrite, single walled nanotube, Viability assay, Cytotoxicity, nitrite, Barrier function, multi walled nanotube, Micronucleus Tests, Nanotubes, Nanotubes, Carbon, inducible nitric oxide synthase, Resazurin, Hydrogen Peroxide, General Medicine, DNA, respiratory system, Comet assay, chemistry, Micronucleus test, Biophysics, Aluminum Silicates, Comet Assay, Micronucleus, Genotoxicity
Abstract

High-aspect-ratio nanomaterials (HARN) (typically, single-walled carbon nanotubes (SWCNT) or multiwalled carbon nanotubes (MWCNT)) impair airway barrier function and are toxic to macrophages. Here, we assess the biological effects of nanotubes of imogolite (INT), a hydrated alumino-silicate [(OH)3Al2O3SiOH] occurring as single-walled NT, on murine macrophages and human airway epithelial cells. Cell viability was assessed with resazurin. RT-PCR was used to study the expression of Nos2 and Arg1, markers of classical or alternative macrophage activation, respectively, and nitrite concentration in the medium was determined to assess NO production. Epithelial barrier integrity was evaluated from the trans-epithelial electrical resistance (TEER). Potential genotoxicity of INT was assessed with comet and cytokinesis-block micronucleus cytome assays. Compared to MWCNT and SWCNT, INT caused much smaller effects on RAW264.7 and MH-S macrophage viability. The incubation of macrophages with INT at doses as high as 120 μg/cm(2) for 72 h did not alter either Nos2 or Arg1 expression nor did it increase NO production, whereas IL6 was induced in RAW264.7 cells but not in MH-S cells. INT did not show any genotoxic effect in RAW264.7 and A549 cells except for a decrease in DNA integrity observed in epithelial A549 cells after treatment with the highest dose (80 μg/cm(2)). No significant change in permeability was recorded in Calu-3 epithelial cell monolayers exposed to INT, whereas comparable doses of both SWCNT and MWCNT lowered TEER. Thus, in spite of their fibrous nature, INT appear not to be markedly toxic for in vitro models of lung-blood barrier cells.

Published
2014

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