Développement méthodologique en FT-ICR MS pour l'analyse de bio-huiles issue de la pyrolyse de la biomasse lignocellulosique
Rapporteurs : | Mme Laurence CHARLES | Pr, ICR, Université Aix-Marseille |
Mme Nadège CHARON | IGR, IPF Energies Nouvelles | |
Examinateurs : | Mme Marie HUBERT-ROUX | IGR, COBRA, Université de Rouen |
M. Yann LE BRECH | MCF, LRGP, Universite de Lorraine | |
M. Guillaume VAN DER REST | Pr, ICP, Université de Paris Saclay | |
Présidente du jury : | Mme Stéphanie HESSE | Pr, LCP-A2MC, Université de Lorraine |
Directeurs de thèse : | M. Frédéric AUBRIET | Pr, LCP-A2MC, Université de Lorraine |
M. Vincent CARRÉ | MCF, LCP-A2MC, Université de Lorraine |
Lieu : ISEA, 7 Rue Marconi, 57070 Metz - Salle Amphithéâtre à 9h00
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Bio-oils from lignocellulosic biomass are promising sources for producing biofuels and high-added-value chemicals. Different processes, such as pyrolysis, allow the conversion of lignocellulosic biomass into bio-oils. The composition of these bio-oils is complex and contains highly oxygenated compounds, which limits their use. Therefore, these bio-oils must be upgraded by catalytic deoxygenation and/or cracking treatments. To determine the effectiveness of the catalytic treatments, a thorough knowledge of the chemical composition of bio-oils is required. A high-resolution mass spectrometer, such as Fourier Transform Ion Cyclotron Resonance (FT-ICR MS) coupled with ESI, APPI, and APCI, allows for in-depth study of the composition of the generated bio-oil at the molecular level. To evaluate the chemical characteristics of these compounds, the research conducted in this PhD thesis focuses on two aspects. The first is based on developing an analytical fractionation/derivatization method to label oxygen-containing compounds according to their functional groups. Combining solid-phase extraction (SPE) with an anion exchange sorbent and derivatization with stable isotope-labeled agents demonstrated, the identification of several oxygenated classes of bio-oil constituents by FT-ICR MS analyses. The second aspect is applied for the first time to bio-oil analysis. It uses two-dimensional ultraviolet photodissociation mass spectrometry (UVPD-MS) for structural analysis of the bio-oil components. Without using the conventional precursor ion isolation and fragmentation for MS/MS experiment, 2D-UVPD-MS has proven to be a powerful tool for performing tandem mass spectrometry experiments on such a complex system. 2D-UVPD-MS has showed to efficiently fragment small, single-charged molecules and to produce fragment ions from various chemical species, such as bio-oil components, thus providing useful structural information.