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

Periodic Reporting for period 1 - BioELCell (Bioproducts Engineered from Lignocelluloses: from plants and upcycling to next generation materials)

Reporting period: 2018-08-01 to 2020-01-31

BioElCell investigates groundbreaking approaches to create next material generation 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 bioeconomy of the future, critically important to Europe and the world.
BioElCell project, led by Prof. Orlando Rojas, Aalto University, Finland, 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 tackles directly or indirectly the grand challenges for engineering, namely, water use, carbon sequestration, nitrogen cycle, food and advanced materials. Indeed, BioElCell studies the key fundamental elements of the research lines, proposes rational use of plant-based materials as a sustainable resource and makes possible the generation of new functions and advanced materials.
BioElCell goes far beyond what is known today about cellulose and lignin micro and nanoparticles, some of the most promising materials of our century, which are emerging and key elements for the success of the future, sustainable society.
BioELCell used plant fibers as sources of originating cellulose nanofibers and nanocrystals. Lignins from pulp and paper processes were used as feedstock for the manufacture of colloidal lignin or lignin micro- and nanoparticles. BioELCell embarked in studies related to marine biomass, including the generation of chitin nanofiber and nanocrystals as well as biobased polyaromatic particles, such as those derived from tannins.
Particle-based membrane combining lignin particles and cellulose nanofibrils is introduced. The synergies inherent to lignin and cellulose in plants were re-engineered to render materials with low surface energy and were rendered 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.
We achieve 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.
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. For potential uses in cardiac devices, the interactions of the scaffolds with cardiac myoblast cells was demonstrated with attachment, proliferation, and viability.
Cellulose nanofibrils (CNF) were introduced for the preparation of scaffolds taking advantage of their biocompatibility and ability to form strong 3D porous networks from aqueous suspensions. Bioactive CNF with interconnected 3D networks for bone formation were prepared through a simple and scalable strategy.
Liquid crystalline phase transitions in aqueous dispersions of high strength cellulose nanocrystals (CNCs) were retained in chiral-nematic ordered aerogels of controlled meso- and microstructures and with improved mechanical properties.
Controlling capillary stresses arising during CNC assembly on meshed architecture was shown to enable control over the orientation of the chiral-nematic director across the topography of the template. Ongoing work on controlling the nematic liquid crystalline phase of ChNCs is a necessity to fully benefit from nanoparticle anisotropy and induced long-range order facilitating fiber spinning.
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.
BioELCell expected further progress in biomedical applications of CNF-based scaffolds, for example, for bone formation, as 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.
BioELCell demonstrated lignin nanoparticle coatings and films with tunable structure by adjusting the drying conditions. This provides a first insight into the possibilities of using polydisperse lignin particle-based systems for applications in coatings, catalysis, barrier materials, flexible electronics.
BioELCell 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 has been shown to enable next generation organic actuators, sensors, resonators and devices for energy harvesting via anisotropic nanoparticle piezoelectric properties, to date not fully understood for cellulose nanocrystals.
Functional 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.
We have effectively demonstrated cellulose nanofibrils as universal binders for MNL and biogenic silica. Several supracolloidal designs have been achieved.
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. The performance of acetylated nanocellulose bioinks opens the possibility for reliable and scaleup fabrication of scaffolds appropriate for studies on cellular processes and for tissue engineering.
Summary for BioElCell research