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Thermally insulating foams and aerogels based on cellulose nanofibrils (CNFs) are promising alternatives to fossil-based thermal insulation materials. We demonstrate a scalable route for moisture-resilient lightweight foams that relies on sclerotization-inspired Michael-type cross-linking of amine-modified CNFs by oxidized tannic acid. The solvent-exchanged, ice-templated, and quinone-tanned cross-linked anisotropic structures were mechanically stable and could withstand evaporative drying with minimal structural change. The low-density (7.7 kg m–3) cross-linked anisotropic foams were moisture-resilient and displayed a compressive modulus of 90 kPa at 98% relative humidity (RH) and thermal conductivity values close to that of air between 20 and 80% RH at room temperature. Sclerotization-inspired cross-linking of biobased foams offers an energy-efficient and scalable route to produce sustainable and moisture-resilient lightweight materials., Moisture-stable and thermally insulating biobased foams were produced using nature-inspired, cross-linking, and energy-efficient evaporative drying.

Nanocellulose-based materials and nanocomposites show extraordinary mechanical properties with high stiffness, strength, and toughness. Although the last decade has witnessed great progress in understanding the mechanical properties of these materials, a crucial challenge is to identify pathways to introduce high wet strength, which is a critical parameter for commercial applications. Because of the waterborne fabrication methods, nanocellulose-based materials are prone to swelling by both adsorption of moist air or liquid water. Unfortunately, there is currently no best practice on how to take the swelling into account when reporting mechanical properties at different relative humidity or when measuring the mechanical properties of fully hydrated materials. This limits and in parts fully prevents comparisons between different studies. We review current approaches and propose a best practice for measuring and reporting mechanical properties of wet nanocellulose-based materials, highlighting the importance of swelling and the correlation between mechanical properties and volume expansion.

The mechanical performance in the wet state needs to be significantly improved and the intrinsic functionalities should be fully utilized to promote the replacement of fossil-based plastics with renewable biobased materials. We demonstrate a leather-inspired approach to produce multifunctional materials with a high wet strength that is based on tannin-induced precipitation of gelatin grafted onto surface-modified cellulose nanofibrils (CNF). The leather-inspired CNF-based films had a wet tensile strength of 33 MPa, a Young’s modulus of 310 MPa, and a strain at failure of 22%, making the wet materials stronger than, for example, dry conventional low-density polyethylene and more ductile than paper-based food packaging materials. The tannin-containing films displayed excellent antioxidant and UV-blocking properties, rapidly scavenging more than 90% of added free radicals and absorbing 100% of light in the UV-B/UV-C range. This work illustrates the prospect of combining renewable materials in a leather-inspired approach to form wet strong and multifunctional films with potential application in food packaging.

Inspired by the Bogolanfini dyeing technique, we report how flexible nanofibrillated cellulose (CNF) films can be functionalized and patterned by surface-bound nanoparticles of hydrolyzable tannins and multivalent metal ions with tunable colors. Molecular dynamics simulations show that gallic acid (GA) and ellagic acid (EA) rapidly adsorb and assemble on the CNF surface, and atomic force microscopy confirms that nanosized GA assemblies cover the surface of the CNF. CNF films were patterned with tannin-metal ion nanoparticles by an in-fibre reaction between the pre-impregnated tannin and the metal ions in the printing ink. Spectroscopic studies show that the Fe-III/II ions interact with GA and form surface-bound, stable GA-Fe-III/II nanoparticles. The functionalization and patterning of CNF films with metal ion-hydrolyzable tannin nanoparticles is a versatile route to functionalize films based on renewable materials and of interest for biomedical and environmental applications.

Cellulose nanofibrils (CNFs) are a unique nanomaterial because of their abundant, renewable, and biocompatible origin. Compared with synthetic nanoparticles, CNFs are commonly produced from cellulose fibers (e.g., wood pulp) by repetitive high-shear mechanical disintegration. Yet, this process is still highly demanding in energy and costly, slowing down the large-scale production and commercialization of CNFs. Reducing the energy consumption during fibers fibrillation without using any chemical or enzymatic pretreat- ments while sustaining the CNF quality is challenging. Here, we show that the anisotropic properties of the CNF foams are directly connected to the degree of nanofibrillation of the cellulose fibers. CNFs were produced from wood pulps using a grinder at increasing specific energy consumptions. The anisotropic CNF foams were made by directional ice templating. The porous architecture, the compressive behavior of the foams, and the CNF alignment in the foam cell walls were correlated to the degree of fibrillation. A particular value of specific energy consumption was identified with respect to the highest obtained foam properties and CNF alignment. This value indicated that the optimal degree of fibrillation, and thus CNF quality, was achieved for the studied cellulose pulp. Our approach is a straightforward tool to evaluate the CNF quality and a promising method for the benchmarking of different CNF grades.