Doctoral thesis (Dissertations and theses)
Editing sustainable (and circular) polymers from co2 and renewables
Siragusa, Fabiana
2022
 

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Keywords :
carbon dioxide; polyurethane; polycarbonate; Chemical recycling
Abstract :
[en] Among all materials, plastics have become one of the most important products of our daily life. Thanks to their ease of production and processing, low cost and customizable properties, plastics are indeed found in pretty much all sectors with applications, for example, in packaging, automotive, pharmaceutical industries or for electrical and electronical devices. However, they are mainly produced from petroleum and contaminate the environment when not properly recycled, which leads to the environmental disaster that we all know. The utilization of carbon dioxide (CO2) as a substitute to petroleum is expected to limit our dependency to this depleting fossil resource and to avoid to be dramatically affected by the associated geopolitical issues that we are currently facing. CO2 is indeed available at large quantities and low cost, and it might contribute to a more sustainable plastic sector by enabling the on-site production of plastics. To reach this ambitious goal, efficient transformations operating under mild conditions and producing limited waste have to be developed, and end- of-life scenarios of the new polymers have to be considered. In this perspective, the aim of this PhD thesis is to merge innovative CO2 transformations with bio-based molecules to produce functional polymers under mild conditions. This work was carried out in the framework of the Excellence of Science (EoS) “BIOFACT” project that deals with the transformation of lignin into high-value chemicals and polymers, starting with the very challenging selective depolymerization of lignin. My contribution to this project was to develop innovative routes to copolymerize a variety of lignin- (or sugar)-based diols or diamines with novel highly reactive CO2-based cyclic carbonates with the objective to produce non- phosgene-based polycarbonates (with diols) and non-isocyanate-based polyurethanes (with diamines) at room temperature. The influence of the structure of the amine/alcohol and reaction conditions on the polymer structure and its thermal properties was investigated. With the aim of circular economy in mind, special attention was also devoted to the exploration of end-of-life options for the CO2-based polymers by investigating chemical degradations via solvolysis or via novel approaches of polymers skeletal-editing.
Research center :
Center for Education and Research on Macromolecules (CERM)
Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit
Disciplines :
Materials science & engineering
Chemistry
Author, co-author :
Siragusa, Fabiana  ;  University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium ; University of Bruxelles ( ULB )
Language :
English
Title :
Editing sustainable (and circular) polymers from co2 and renewables
Defense date :
08 December 2022
Number of pages :
302
Institution :
ULiège - University of Liège [Sciences], Liege, Belgium
ULB - Université Libre de Bruxelles [Sciences], Bruxelles, Belgium
Degree :
Doctorate Degree in Science
Promotor :
Detrembleur, Christophe ;  University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium
Evano Gwilherm;  Université de Bruxelles (ULB )
President :
Jérôme, Christine  ;  University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium
Secretary :
Geerts Yves;  University of Bruxelles (ULB )
Jury member :
Odelius Karin;  Royal Institute of Technology, Stockholm, Sweden
Gohy Jean-François;  Universté Catholique de Louvain-la-Neuve (UCL)
Hoogenboom Richard;  Universty of Gent (UGENT)
Funders :
F.R.S.-FNRS - Fund for Scientific Research [BE]
FWO - Flemish Research Foundation [BE]
EOS - The Excellence Of Science Program [BE]
Available on ORBi :
since 15 December 2022

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