Andrea Lazzarini

Andrea Lazzarini
Università degli Studi dell'Aquila | Università dell'Aquila · Department of Physical and Chemical Sciences

Doctor of Philosophy
Oxidation of olefinic double bonds in liquid phase with magnetic catalysts; CO oxidation with ceria-based catalysts

About

42
Publications
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962
Citations
Additional affiliations
March 2013 - December 2016
Università degli Studi di Torino
Position
  • PhD Student

Publications

Publications (42)
Article
the development of novel and more efficient contrast agents for diagnostic applications is necessary to lower the dosage of such substances that might accumulate in patients with toxic effects and to define new agents which effect could go beyond the simplified scheme of T1 or T2 relaxation properties. Within this context, novel directions for MRI...
Article
Clean water is vital for healthy ecosystems, for human life and, in a broader sense, it is directly linked to our socio-economic development. Nevertheless, climate change, pollution and increasing world population will likely make clean water scarcer in the near future. Consequently, it becomes imperative to develop novel materials and more efficie...
Article
The preparation of three novel active and stable magnetic nanocatalysts for the selective liquid-phase oxidation of several olefins, has been reported. The heterogeneous systems are based on the coordination of cis-MoO2 moiety onto three different SCMNP@Si-(L1-L3) magnetically active supports, functionalized with silylated acylpyrazolonate ligands...
Article
Full-text available
Heterogeneous catalysts are progressively expanding their field of application, from high-throughput reactions for traditional industrial chemistry with production volumes reaching millions of tons per year, a sector in which they are key players, to more niche applications for the production of fine chemicals. These novel applications require a pr...
Article
Full-text available
Symmetry breaking is observed in the Soai reaction in a confinement environment provide by zirconium‐based UiO‐MOFs used as crystalline sponges. Subsequent reaction of encapsulated Soai aldehyde with Zn(i‐Pr) 2 vapour promoted absolute asymmetric synthesis of the corresponding alkanol. ATR‐IR and NMR confirm integration of aldehyde into the porous...
Article
Silica-coated iron oxide magnetic nanoparticles to be employed as the starting core for easily-recoverable heterogeneous catalysts supports, were synthesized. We tuned both the properties of the magnetic core and of the covering shell, with particular emphasis on the optimization of the silica layer thickness. Afterwards, structural-sensitive techn...
Article
The main analytical techniques useful for the comprehensive chemical characterization of relevant specimens available from extraterrestrial sample return missions, also considering, among others, the instrumental facilities available at the "Centro di Microscopie" of the University of L'Aquila (UnivAQ), are described. Different qualitative and/or q...
Preprint
We report a novel vapour phase procedure to perform the Soai reaction in an absolute asymmetric synthesis fashion: the substrate is confined in the pores of the UiO-type MOFs, and vapour phase reactions with Zn(i-Pr)<sub>2</sub> are performed in a sealed environment, Different MOFs lead to different outcomes in terms of enantiomeric excess, handedn...
Article
Full-text available
In catalysts for CO2 hydrogenation, the interface between metal nanoparticles (NPs) and the support material is of high importance for the activity and reaction selectivity. In Pt NP-containing UiO Zr-metal-organic frameworks (MOFs), key intermediates in methanol formation are adsorbed at open Zr-sites at the Pt-MOF interface. In this study, we inv...
Article
A challenge in converting CO2 into hydrocarbons (HC) via methanol (MeOH) is the gap between the optimal temperature for each step (i.e. ≤250 °C for MeOH and ≥350 °C for HC). The focus of this study is to elucidate the cause of the limitations associated to oxygenate and hydrocarbon formation in combined PdZn and H-ZSM-5 catalysts at 250 to 350 °C....
Article
Full-text available
Reactions between alkenes and methanol or dimethyl ether (DME) on zeolite catalysts are involved in industrial processes that are highly relevant for the transition to renewable carbon sources, such as the Methanol-To-Hydrocarbons (MTH) process. In MTH chemistry, alkene methylation increases the length of product carbon chains, and its relative rat...
Article
Full-text available
Ni functionalized metal organic frameworks (MOF) are promising heterogeneous ethene dimerization catalysts. Activities comparable to or higher than Ni-aluminosilicates have been reported in literature. However, unlike the Ni-aluminosilicates, those Ni-MOFs require a large excess of co-catalyst to initiate the dimerization process and some catalysts...
Article
Full-text available
Metal-organic frameworks (MOFs) show great prospect as catalysts and catalyst support materials. Yet, studies that address their dynamic, kinetic and mechanistic role in target reactions are scarce. In this study, an exceptionally stable MOF catalyst consisting of Pt nanoparticles (NPs) embedded in a Zr-based UiO-67 MOF was subject to steady-state...
Article
Coke formation is a major reason in deactivation of acidic zeolite catalysts in industrial processes such as methanol to hydrocarbons conversion. Protecting the surface of acidic zeolite with an inert porous shell can greatly hinder the coke formation on the surface, and hence boost the lifetime of the catalyst. In this work, a solid-state steam-as...
Article
Full-text available
The direct stepwise transformation of CH4 to CH3OH over Cu-exchanged zeolites has been an intensively researched reaction as it can provide a solution for the utilization of this abundant feedstock. Up to date a commercial process is far from realization, which is why an understanding of the Cu speciation in zeolites as a function of reaction condi...
Article
This contribution clarifies the overoxidation‐preventing key step in the methane‐to‐methanol (MTM) conversion over copper mordenite zeolites. We followed the methane‐to‐methanol conversion over copper mordenite zeolites by NMR supported by DRIFTS to show that surface methoxy groups (SMGs) located at zeolite Brønsted sites are the key intermediates....
Article
The successful synthesis of metal-organic framework (MOF) compounds relies on an intricate interplay between the compo-nents of the synthesis liquor at the given synthesis conditions. Herein, we explore the interdependence of modulator, linker and solvent amounts in the synthesis of the Zr-based MOF, UiO-67. Our study suggests that control of linke...
Article
We report a complete experimental characterization of the surface Pt-hydride species on an industrial 5wt% Pt/Al2O3 catalyst (average particle size of 1.4 ± 0.4 nm) under different hydrogenation/dehydrogenation conditions. By combining Inelastic Neutron Scattering, FT-IR spectroscopy and synchronous DRIFT/XAS/MS, we identified n-fold coordinated Pt...
Article
Functionalization of metal-organic frameworks (MOFs) with noble metals is a promising way for producing new versatile catalysts that will combine the outstanding porosity and specific surface area of MOFs with high catalytic activity of metals. Here, we present a comparative study of two metal-organic frameworks with UiO-67 topology, functionalized...
Article
The behaviour of a Pd(OAc)2/P4VP catalyst submitted to different pre-treatments (pre-reduced, pre-oxidised and un-treated) during the aerobic oxidation of 2-propanol to acetone in the gas phase has been investigated. Synchronous, time-resolved, SAXS/XAS/MS techniques coupled with operando DRIFT spectroscopy (which gave information on the destiny of...
Article
Functionalization of metal-organic frameworks with metal nanoparticles (NPs) is a promising way for producing advanced materials for catalytic applications. We present synthesis and in situ characterization of palladium NPs encapsulated inside functionalized UiO-67 metal-organic framework. The initial structure was synthesized with 10% of PdCl2bpyd...
Article
Formation of palladium hydride and carbide phases in palladium-based catalysts is a critical process which changes the catalytic performance and selectivity of the catalysts in important industrial reactions, such as selective hydrogenation of alkynes or alkadienes. We present a comprehensive study of a 5 wt.% carbon supported Pd nanoparticles (NPs...
Article
We looked at the active hydrogen species in a highly dispersed and very homogeneous 5wt% Pt/C industrial catalyst (Pt particle mean diameter of 2.0 ± 0.5 nm) for hydrogenation reactions, by coupling H2 adsorption measurements with Inelatic Neutron Scattering (INS). Taking advantage of the enormous progresses undergone by the INS instruments, we suc...
Article
Substituting metals for either aluminum or phosphorus in crystalline, microporous aluminophosphates creates Brønsted acid sites, which are well known to catalyze several key reactions, including the methanol to hydrocarbons (MTH) reaction. In this work, we synthesized a series of metal-substituted aluminophosphates with AFI topology that differed p...
Article
Full-text available
The synthesis, characterization and catalytic performance of offretite with four distinct crystal morphologies (oval, hexagonal, broccoli-like, spherical) are presented. As a member of the ABC-6 family of zeolite structures, offretite is likely to form intergrowths which can affect shape-selective properties. Herein, the combination of experiments...
Article
Full-text available
In this work we investigated in details the effects of nitric acid on the surface chemistry of two carbons, activated by steam and by phosphoric acid, meant to identify the nature and the concentration of the oxidized surface species. To this aim, the oxidized carbons were characterized by means of a large number of complementary techniques, includ...
Article
Full-text available
CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220–280 °C and ambient pressure, with H2/CO2 = 0.2–9 and contact times, τ = 0.004–0.01 gcat×min×ml−1. The catalysts were characterized by XRD, N2 adsorption, FESEM, TEM and HRTEM, dissolution-NMR, CO chemisorption, IR spectroscopy and TGA. A positive correlation was observed...
Article
We report an in situ, temperature and H2 pressure-dependent, characterization of (2.6  0.4) nm palladium nanoparticles supported on active carbon during the process of hydride phase formation. For the first time the core-shell structure is highlighted in the single-component particles on the basis of a different atomic structure and electronic con...
Article
This paper is a concise review on the principal physical–chemical techniques available to investigate the structural and surface properties of activated carbons (ACs) for catalytic applications. The same AC has been characterized by an incredible amount of techniques: Solid state-nuclear magnetic resonance, X-ray powder diffraction and Raman spectr...
Article
Full-text available
The effect of a graphitization treatment on the phyisico-chemical properties of an activated carbon have been studied by means of multi-technical approach. Inelastic neutron scattering and DRIFT spectroscopy revealed the modifications occurring at the material borders, involving H-containing species and O-containing functional groups. Information o...
Article
Full-text available
Simultaneous time-resolved SAXS and XANES techniques were employed to follow in situ the formation of Pd nanoparticles from palladium acetate precursor in two porous polymeric supports: polystyrene (PS) and poly(4-vinyl-pyridine) (P4VP). In this study we have investigated the effect of the use of different reducing agents (H2 and CO) from the gas p...
Article
In the current work we present a detailed analysis of the hydride phase formation in industrial Pd/C nanocatalysts by means of combined in situ X-ray absorption spectroscopy (EXAFS), X-ray diffraction (XRD) and volumetric measurements for the temperatures from - 10 to 50 °C in the hydrogen pressure range from 0 to 1000 mbar. α- and β- hydride phase...
Article
Full-text available
Activated carbons are widely used as supports for industrial catalysts based on metal nanoparticles. The catalytic performances of carbon-supported catalysts are strongly influenced by the carbon activation method. Notwithstanding this important role, the effect induced by different activation methods have been rarely invesigated in details. This w...
Article
Full-text available
Activated carbons are materials with relevance in different industrial applications. Due to the inherent complexity and heterogeneity of their structures, an easy assignment of the species present on their surface has a challenging result. Only recently, with the possibility to collect well-resolved inelastic neutron spectra and to simulate by DFT...
Article
The reactivity of palladium acetate inside a poly(4-vinylpyridine-co-divinylbenzene) polymer is strongly influenced by the establishment of interaction between the Pd precursor and the pyridyl functional group in the polymer. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and simultaneous X-ray absorption near edge structure (...
Article
In the typical NH3-SCR temperature range (100–500 °C), ammonia is one of the main adsorbed species on acidic sites of Cu-SSZ-13 catalyst. Therefore the study of adsorbed ammonia at high temperature is a key step for the understanding of its role in the NH3-SCR catalytic cycle. We employed different spectroscopic techniques in order to investigate t...

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Project (1)
Project
This project is being worked intensively in collaboration between several research groups from the Southern Federal University (Russia), University of Turin and Chimet company (Italy), ETH Zurich and Swiss Light Source (Switzerland), ESRF (France), and some others. We study different palladium-based catalysts (mostly supported nanoparticles) by synchrotron-based techniques, X-ray absorption spectroscopy being most actively applied. These studies include both fundamental investigation of phase transitions and kinetics of formation of palladium hydrides, carbides and oxides, and more applied operando studies of real industrial catalysts under relevant working conditions. For those who don't like reading papers - watch this funny video that was submitted for Dance Your PhD contest of the Science Magazines: https://www.youtube.com/watch?v=eQwk9fkJXDU