Periodic Reporting for period 3 - BioELCell (Bioproducts Engineered from Lignocelluloses: from plants and upcycling to next generation materials) Reporting period: 2021-08-01 to 2023-01-31 Summary of the context and overall objectives of the project BioElCell investigates groundbreaking approaches to create materials based on renewable resources, mainly cellulose and lignin micro- and nanoparticles. Our action disassembles and re-engineers plant-based polymers into functional materials that will respond to the demands of the future bioeconomy, critically important to Europe and the world.BioElCell uses multiphase systems with ultra-low interfacial tension to facilitate nanocellulose liberation and atomization of lignin solution streams into spherical particles. BioElCell designs novel routes to control the reassembly of the respective particles in new 1-D, 2-D and 3-D structures. The systematic methodologies address the main challenges for lignocellulose processing and deployment, considering the interactions with water. BioElCell presents a transformative approach by integrating complementary disciplines that lead to a far-reaching understanding of lignocellulosic biopolymers and solve key challenges in their use, paving the way to functional product development.Results obtained from BioElCell tackle the grand challenges for engineering, namely, water use, carbon sequestration, nitrogen cycle, food, and advanced materials. BioElCell goes far beyond what is known today about cellulose and lignin micro and nanoparticles, which are emerging and key elements for the success of the future, sustainable society. Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far Particle-based membrane from lignin particles and cellulose nanofibers (CNFs) is introduced for materials with low surface energy and water-resistance with the aid of wet-strength agents. Electron tomography method was employed for colloidal interactions and produced tomography-based 3D models of wrinkled colloidal lignin particles. Oxygen, water vapor, and UV barriers were achieved using a stepwise layered assembly of CNFs, biobased wax, and lignin particles supported by chitin nanofibers.CNF networks enabled universal assembly of super-structured particle constructs. We achieved biogenic silica nanoparticle structuring into controlled morphologies together with CNFs, promoting cohesion in green 3D supraparticle formation. Cargo loading/unloading of a model, green biomolecule (thymol), and for photo accessibility and mobility in soil was evaluated. We introduce CNFs as a reinforcing agent to tannin foams that eliminates the need for chemical crosslinking during foam formation.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.Extremely effective Pickering emulsion stabilizers were prepared from complexed cellulose nanocrystals (CNC) and nanochitin.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. 3D-printed scaffolds from multiphase systems were applied in nanocellulosic materials for bone regeneration. 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 aerogels of controlled meso- and microstructures and with improved mechanical properties. CNCs produced remarkable anisotropic adhesive strength with anisotropic adhesion.Cationic and anionic cellulose nanoparticles were used to control protein interactions on surfaces. Polyphenol-based particles with a variety of tailorable morphologies were produced from tannic acid using a facile synthesis method.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. Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far) BioELCell progress impacts on biomedical applications 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 can be envisioned to form new ranges of lightweight yet extremely strong and tough materials matching biological architectures. CNCs induce extremely high, noncovalent adhesive shear strength as fully green, cost‐effective, and aqueous‐based bio adhesive for reversible supergluing. BioELCell will deliver improved bio-based adhesive formulations.BioELCell demonstrated lignin nanoparticle coatings, membranes, and films with tunable structure by adjusting the drying conditions and multilayering. This provides a first insight into using polydisperse lignin particle-based systems for applications in coatings, catalysis, barrier materials, flexible electronics.CNFs were demonstrated as universal binders for micro/nanolignin MNL and biogenic silica. Several supracolloidal designs have been achieved through superstructuring of virtually any particle with CNF networks. We are developing platforms for carbon capture utilizing superstructuring with CNFs.BioELCell project will explore 1D filaments based on micro/nanocellulose (MNC) and nanochitin originating from crab/shrimp shell residuals as well as those produced from fungi and insects. Fibers can be conveniently modified to install conductive, magnetic, phase change, heating, and thermo-chromic features.Functional 2D coatings and films will enable flexible electronics with special properties at surface and bulk levels, such as conductivity, (super)hydrophobicity/hydrophilicity, transparency, tailorable porosity, and magnetic shielding for uses as active component in multiple types of electronic devices. Inkjet-printed cellulose nanospheres on patterned immunoassays enabled rapid and sensitive SARS-CoV-2 nucleocapsid detection.Foams and emulsions as multiphase systems are expected to become critical in the synthesis of next generation 3D printed materials and to facilitate structural and functional food. Direct ink writing (DIW) with two-phase emulgels including cellulose-and chitin nanoparticles provided programmable and customizable platforms to engineer hierarchically organized constructs via 3D printing. We demonstrated the concept of dynamic supramolecular hydrogel-reinforced emulgels to overcome the significant limitations of DIW of Pickering emulsions with undesirable rheological properties. Acetylated nanocellulose bio inks open the possibility for reliable and scaleup fabrication of scaffolds for cellular processes and for tissue engineering. Green and sustainable CNF-reinforced tannin foams for insulation are, stronger, lighter, and more resistant to fire compared to those produced by formaldehyde crosslinking. Summary for BioElCell research
