Periodic Reporting for period 4 - BioELCell (Bioproducts Engineered from Lignocelluloses: from plants and upcycling to next generation materials)
Période du rapport: 2023-02-01 au 2023-07-31
BioElCell investigated groundbreaking approaches to create materials based on renewable resources, mainly cellulose and lignin micro- and nanomaterials. Our action disassembled and re-engineered plant-based polymers into functional systems that are suited to respond to the demands of the future bioeconomy, critically important to Europe and the world.
BioElCell used multiphase systems with ultra-low interfacial tension to facilitate nanocellulose liberation and atomization of lignin streams into spherical particles. The program also designed novel routes to control the reassembly of the respective particles into new 1-D, 2-D and 3-D structures. The systematic methodologies advanced by BioELCell will address some of the main challenges for lignocellulose processing and deployment, considering the interactions with water. BioElCell presented a transformative approach by integrating complementary disciplines that is leading to a far-reaching understanding of lignocellulosic biopolymers and solve key challenges in their use, for instance, considering energy and water demands, carbon sequestration, nitrogen cycle, food, and accessibility to raw materials. BioElCell positioned cellulose and lignin structures as emerging elements for the success of a sustainable society.
BioElCell used multiphase systems with ultra-low interfacial tension to facilitate nanocellulose liberation and atomization of lignin streams into spherical particles. The program also designed novel routes to control the reassembly of the respective particles into new 1-D, 2-D and 3-D structures. The systematic methodologies advanced by BioELCell will address some of the main challenges for lignocellulose processing and deployment, considering the interactions with water. BioElCell presented a transformative approach by integrating complementary disciplines that is leading to a far-reaching understanding of lignocellulosic biopolymers and solve key challenges in their use, for instance, considering energy and water demands, carbon sequestration, nitrogen cycle, food, and accessibility to raw materials. BioElCell positioned cellulose and lignin structures as emerging elements for the success of a sustainable society.
Particle-based membranes based on lignin particles and cellulose nanofibers (CNF) were designed to exhibit low surface energy and water-resistance. Methods to measure interactions forces (AFM) and imaging (electron tomography and others) were employed to understand colloidal forces and to produce 3D models of wrinkled colloidal lignin particles. Oxygen, water vapor, and UV barriers were achieved using a stepwise layered assembly of CNF, biobased wax, and lignin particles supported by chitin nanofibers.
Networks based on cellulose fibrils (CNF) enabled universal assembly of super-structured particle constructs. We structured nanoparticles (biogenic silica, organic and biological particles of different charges and surface energy) into controlled morphologies supported by CNF, promoting cohesion in green 3D supraparticle formation. Cargo loading/unloading of biomolecules (thymol and others), and photo accessibility and mobility in soil were evaluated. We introduced CNFs as a reinforcing agent in tannin foams that eliminated the need for chemical crosslinking during foam formation. In other efforts, involving liquid multiphases, BioELCell achieved extremely stable Pickering emulsion by using biocolloid stabilization (from complexed cellulose nanocrystals (CNC) and nanochitin).
Wet spinning in a coaxial configuration was used in extruding oxidized nanocellulose combined with airflow in the core. The coagulation of the produced hydrogel resulted in hollow filaments used for phase change materials with proper infills. Other extrusion based technologies were introduced. For instance, aqueous suspensions of acetylated nanocellulose were used for 3D printing of bio scaffolds. The interactions of the scaffolds with cardiac myoblast cells were demonstrated with attachment, proliferation, and viability. The 3D-printed scaffolds from multiphase systems were applied in nanocellulosic materials for bone regeneration. Finally, a supramolecular host-guest hydrogel based on poly(ethylene glycol) and a-cyclodextrin was synthesized in the continuous phase of CNC stabilized Pickering emulsion for direct ink writing. Implantable meshes with auxetic structures were prepared from bacterial nanocellulose using solid supports guiding the biofilm formation.
Liquid crystal order in aqueous dispersions of high strength CNCs was retained in chiral-nematic systems of controlled meso- and microstructures and with improved mechanical properties. Surface bound confined water medium was shown to increase chemical reaction rate, efficiency, and selectivity for cellulose hydroxyl group functionalities, essential for optimal utilization of cellulosic nanomaterials. Chitin nanocrystal and protein interactions were harnessed to develop high strength green adhesives. Further developments in the area included the formation of nematic phases, which were demonstrated to produce remarkable anisotropic adhesion strength with aqueous dispersions of CNC. Finally, cationic and anionic cellulose nanoparticles were used to control protein interactions on surfaces and polyphenol-based particles with a variety of tailorable morphologies were produced from tannic acid using a facile synthesis method.
Networks based on cellulose fibrils (CNF) enabled universal assembly of super-structured particle constructs. We structured nanoparticles (biogenic silica, organic and biological particles of different charges and surface energy) into controlled morphologies supported by CNF, promoting cohesion in green 3D supraparticle formation. Cargo loading/unloading of biomolecules (thymol and others), and photo accessibility and mobility in soil were evaluated. We introduced CNFs as a reinforcing agent in tannin foams that eliminated the need for chemical crosslinking during foam formation. In other efforts, involving liquid multiphases, BioELCell achieved extremely stable Pickering emulsion by using biocolloid stabilization (from complexed cellulose nanocrystals (CNC) and nanochitin).
Wet spinning in a coaxial configuration was used in extruding oxidized nanocellulose combined with airflow in the core. The coagulation of the produced hydrogel resulted in hollow filaments used for phase change materials with proper infills. Other extrusion based technologies were introduced. For instance, aqueous suspensions of acetylated nanocellulose were used for 3D printing of bio scaffolds. The interactions of the scaffolds with cardiac myoblast cells were demonstrated with attachment, proliferation, and viability. The 3D-printed scaffolds from multiphase systems were applied in nanocellulosic materials for bone regeneration. Finally, a supramolecular host-guest hydrogel based on poly(ethylene glycol) and a-cyclodextrin was synthesized in the continuous phase of CNC stabilized Pickering emulsion for direct ink writing. Implantable meshes with auxetic structures were prepared from bacterial nanocellulose using solid supports guiding the biofilm formation.
Liquid crystal order in aqueous dispersions of high strength CNCs was retained in chiral-nematic systems of controlled meso- and microstructures and with improved mechanical properties. Surface bound confined water medium was shown to increase chemical reaction rate, efficiency, and selectivity for cellulose hydroxyl group functionalities, essential for optimal utilization of cellulosic nanomaterials. Chitin nanocrystal and protein interactions were harnessed to develop high strength green adhesives. Further developments in the area included the formation of nematic phases, which were demonstrated to produce remarkable anisotropic adhesion strength with aqueous dispersions of CNC. Finally, cationic and anionic cellulose nanoparticles were used to control protein interactions on surfaces and polyphenol-based particles with a variety of tailorable morphologies were produced from tannic acid using a facile synthesis method.
BioELCell impact on biomedical applications is paving the way towards a facile preparation of advanced, high-performance CNF-based scaffolds for bone tissue engineering. Cellulose nanocrystal (CNC) self-assembly and chiral nematic structure formation was studied simultaneously via tessellation at nano- and macrostructure levels. A combination of cellular metamaterials and long-range ordered nanoparticle composites were achieved. They will form new ranges of lightweight yet extremely strong and tough materials matching biological architectures. CNC was shown to induce extremely high, noncovalent adhesive shear strength in a fully green, cost‐effective, and aqueous‐based bio adhesive.
BioELCell demonstrated lignin nanoparticle coatings, membranes, and films with tunable structure by adjusting the drying conditions and multilayering. This provides a first insight into polydisperse lignin particle-based systems for applications in coatings, catalysis, barrier materials and flexible electronics.
CNFs were demonstrated as universal binders for micro/nanolignin particles and biogenic silica. Several supracolloidal designs were achieved through superstructuring. The CNF-based networks developed were shown to be a generic approach that was demonstrated with a variety of particles. Using similar systems, BioELCell developed platforms for carbon capture via superstructuring with CNFs.
BioELCell project set the goal to develop 1D filaments based on micro/nanocellulose and nanochitin originating from crab/shrimp shell residuals as well as those produced from fungi and insects. Such efforts was highly successful by using wet and dry spinning. Microfiber and filaments were conveniently modified to install conductive, magnetic, phase change, heating, and thermo-chromic features.
Functional 2D coatings and films enabled flexible electronics with special properties at surface and bulk levels, such as conductivity, (super)hydrophobicity/hydrophilicity, transparency, tailorable porosity, and magnetic shielding. These designs were demonstrated as active components in various types of electronic devices. In a recent effort, inkjet-printed cellulose nanospheres were patterned on cellulose films to produce immunoassays for rapid and sensitive SARS-CoV-2 nucleocapsid detection.
Moving to 3D systems, BioELCell produced several breakthroughs in the formulation of foams and emulsions (multiphase systems), which are critical for the synthesis of next generation structured materials. For instance, direct ink writing (DIW) with two-phase emulgels including cellulose-and chitin nanoparticles, provided programmable and customizable platforms to engineer hierarchically organized constructs. We demonstrated the concept of dynamic supramolecular hydrogel-reinforced emulgels to overcome the significant limitations of DIW of Pickering emulsions. Acetylated nanocellulose and lignin nanoparticle bioinks were introduced as means to open the possibility for reliable and scaleup fabrication of scaffolds for cellular processes, tissue engineering and green approaches to traditional printing. Green and sustainable CNF-reinforced tannin foams were also presented for insulation and to endow stronger, lighter, and fire-resistant solution that can replace those produced from EPS and other foams as well as those that require formaldehyde crosslinking.
BioELCell demonstrated lignin nanoparticle coatings, membranes, and films with tunable structure by adjusting the drying conditions and multilayering. This provides a first insight into polydisperse lignin particle-based systems for applications in coatings, catalysis, barrier materials and flexible electronics.
CNFs were demonstrated as universal binders for micro/nanolignin particles and biogenic silica. Several supracolloidal designs were achieved through superstructuring. The CNF-based networks developed were shown to be a generic approach that was demonstrated with a variety of particles. Using similar systems, BioELCell developed platforms for carbon capture via superstructuring with CNFs.
BioELCell project set the goal to develop 1D filaments based on micro/nanocellulose and nanochitin originating from crab/shrimp shell residuals as well as those produced from fungi and insects. Such efforts was highly successful by using wet and dry spinning. Microfiber and filaments were conveniently modified to install conductive, magnetic, phase change, heating, and thermo-chromic features.
Functional 2D coatings and films enabled flexible electronics with special properties at surface and bulk levels, such as conductivity, (super)hydrophobicity/hydrophilicity, transparency, tailorable porosity, and magnetic shielding. These designs were demonstrated as active components in various types of electronic devices. In a recent effort, inkjet-printed cellulose nanospheres were patterned on cellulose films to produce immunoassays for rapid and sensitive SARS-CoV-2 nucleocapsid detection.
Moving to 3D systems, BioELCell produced several breakthroughs in the formulation of foams and emulsions (multiphase systems), which are critical for the synthesis of next generation structured materials. For instance, direct ink writing (DIW) with two-phase emulgels including cellulose-and chitin nanoparticles, provided programmable and customizable platforms to engineer hierarchically organized constructs. We demonstrated the concept of dynamic supramolecular hydrogel-reinforced emulgels to overcome the significant limitations of DIW of Pickering emulsions. Acetylated nanocellulose and lignin nanoparticle bioinks were introduced as means to open the possibility for reliable and scaleup fabrication of scaffolds for cellular processes, tissue engineering and green approaches to traditional printing. Green and sustainable CNF-reinforced tannin foams were also presented for insulation and to endow stronger, lighter, and fire-resistant solution that can replace those produced from EPS and other foams as well as those that require formaldehyde crosslinking.