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Bioproducts Engineered from Lignocelluloses: from plants and upcycling to next generation materials

Periodic Reporting for period 2 - BioELCell (Bioproducts Engineered from Lignocelluloses: from plants and upcycling to next generation materials)

Reporting period: 2020-02-01 to 2021-07-31

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.
Particle-based membrane from lignin particles and cellulose nanofibrils (CNFs) is introduced. The synergies inherent to lignin and cellulose in plants were re-engineered to render materials with low surface energy and were water-resistant with the aid of wet-strength agents. Structured 2D coatings were prepared from polydisperse smooth and spherical biocolloidal lignin particles suspended in aqueous media. Electron tomography method was employed for colloidal interactions and produced tomography-based 3D models of wrinkled colloidal lignin particles.
We presented CNF induced cohesion in particle assemblies. Nanofibrillar networks enabled universal assembly of super-structured particle constructs. We achieved biogenic silica nanoparticle structuring into controlled morphologies together with cellulose nanofibrils, 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 demonstrated superstructuring of virtually any particle.
Two-phase emulgel of 1) a Pickering emulsion with internal phase of poly(lactic acid) stabilized by chitin/cellulose nanofibers and 2) a continuous, cross-linkable hydrogel containing cellulose nanofibers and any of the given solid particles, were used in 3D printing of skin-bearing architectures.
Aqueous suspensions of acetylated nanocellulose of a low degree of substitution were used for 3D printing of bio scaffolds. The interactions of the scaffolds with cardiac myoblast cells was demonstrated with attachment, proliferation, and viability. 3D-printed scaffolds from multiphase systems were applied in nanocellulosic materials for bone regeneration.
Liquid crystal order in aqueous dispersions of high strength cellulose nanocrystals (CNCs) was retained in chiral-nematic aerogels of controlled meso- and microstructures and with improved mechanical properties. Capillary stresses control the orientation of the CNC assembly. CNCs produced remarkable anisotropic adhesive strength with anisotropic adhesion.
Organic solvent-free, heterogeneous, and simple synthesis of spherical carboxylated cellulose nanoparticles bearing a distinctive, amorphous outer shell structure was demonstrated. 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.
BioELCell progresses in biomedical applications of CNF-based scaffolds, for example, for bone formation, are demonstrated by systemic biocompatibility and with no negative effects on vital organs such as the liver and kidneys. We expect to pave the way towards a facile preparation of advanced, high performance CNF-based scaffolds for bone tissue engineering.
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 and films with tunable structure by adjusting the drying conditions. This provides a first insight into using polydisperse lignin particle-based systems for applications in coatings, catalysis, barrier materials, flexible electronics.
We demonstrated cellulose nanofibrils as universal binders for 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 continue to explore 1D filaments for wearable materials 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, heating, and thermo-chromic features. Aligned MNC enables next generation organic actuators, sensors, resonators, and devices for energy harvesting via anisotropic nanoparticle piezoelectric properties, to date not fully understood for CNCs.
Functional coatings and films (2D) 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.
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 with two-phase emulgels including cellulose-and chitin nanoparticles provided programmable and customizable platforms to engineer hierarchically organized constructs via 3D printing. Acetylated nanocellulose bio inks opens the possibility for reliable and scaleup fabrication of scaffolds for cellular processes and for tissue engineering.
Summary for BioElCell research