Gustav Nyström

Self-assembled three-dimensional and compressible interdigitated thin-film supercapacitors and batteries

Traditional thin-film energy-storage devices consist of stacked layers of active films on two-dimensional substrates and do not exploit the third dimension. Fully three-dimensional thin-film devices would allow energy storage in bulk materials with arbitrary form factors and with mechanical properties unique to bulk materials such as compressibility. Here we show three-dimensional energy-storage devices based on layer-by-layer self-assembly of interdigitated thin films on the surface of an open-cell aerogel substrate. We demonstrate a reversibly compressible three-dimensional supercapacitor with carbon nanotube electrodes and a three-dimensional hybrid battery with a copper hexacyanoferrate ion intercalating cathode and a carbon nanotube anode. The three-dimensional supercapacitor shows stable operation over 400 cycles with a capacitance of 25 F g−1 and is fully functional even at compressions up to 75%. Our results demonstrate that layer-by-layer self-assembly inside aerogels is a rapid, precise and scalable route for building high-surface-area 3D thin-film devices.

Understanding nanocellulose chirality and structure-properties relationship at the single fibril level

Nanocellulose fibrils are ubiquitous in nature and nanotechnologies but their mesoscopic structural assembly is not yet fully understood. Here we study the structural features of rod-like cellulose nanoparticles on a single particle level, by applying statistical polymer physics concepts on electron and atomic force microscopy images, and we assess their physical properties via quantitative nanomechanical mapping. We show evidence of right-handed chirality, observed on both bundles and on single fibrils. Statistical analysis of contours from microscopy images shows a non-Gaussian kink angle distribution. This is inconsistent with a structure consisting of alternating amorphous and crystalline domains along the contour and supports process-induced kink formation. The intrinsic mechanical properties of nanocellulose are extracted from nanoindentation and persistence length method for transversal and longitudinal directions, respectively. The structural analysis is pushed to the level of single cellulose polymer chains, and their smallest associated unit with a proposed 2 × 2 chain-packing arrangement.

Nanocellulose Aerogels Functionalized by Rapid Layer‐by‐Layer Assembly for High Charge Storage and Beyond

Step by step: A robust and rapid method for the layer-by-layer assembly of polymers and nanoparticles on strong and elastic aerogels has been developed. Thin films of biomolecules, conducting polym ...

Amyloid Templated Gold Aerogels

Amyloid fibril-based ultralow-density aerogels are designed by functionalization with gold nanoparticles and microcrystals, leading to hybrids of unprecedented lightness and functionality. By changing the colloidal gold shape, size, and concentration, the gold composition can be tuned to reach contents ≥20 kt equivalent, yet at densities ≈10(3) lighter than any equivalent gold alloys, and combining unique features such as porosity, catalytic properties, pressure sensing, and autofluorescence.

Two-Dimensional Aggregation and Semidilute Ordering in Cellulose Nanocrystals

The structural properties and aggregation behavior of carboxymethylated cellulose nanocrystals (CNC-COOH) were analyzed with small angle neutron scattering (SANS), transmission electron microscopy (TEM), atomic force microscopy (AFM), and dynamic light scattering (DLS) and compared to sulfuric acid hydrolyzed cellulose nanocrystals (CNC-SO3H). The CNC-COOH system, prepared from single carboxymethylated cellulose nanofibrils, was shown to laterally aggregate into 2D-stacks that were stable both in bulk solution and when adsorbed to surfaces. CNC-SO3H also showed a 2D aggregate structure with similar cross sectional dimensions (a width to height ratio of 8) as CNC-COOH, but a factor of 2 shorter length. SANS and DLS revealed a reversible ordering of the 2D aggregates under semidilute conditions, and a structure peak was observed for both systems. This indicates an early stage of liquid crystalline arrangement of the crystal aggregates, at concentrations below those assessed using birefringence or polarized optical microscopy.

Amyloid fibril systems reduce, stabilize and deliver bioavailable nanosized iron

Iron-deficiency anaemia (IDA) is a major global public health problem. A sustainable and cost-effective strategy to reduce IDA is iron fortification of foods, but the most bioavailable fortificants cause adverse organoleptic changes in foods. Iron nanoparticles are a promising solution in food matrices, although their tendency to oxidize and rapidly aggregate in solution severely limits their use in fortification. Amyloid fibrils are protein aggregates initially known for their association with neurodegenerative disorders, but recently described in the context of biological functions in living organisms and emerging as unique biomaterial building blocks. Here, we show an original application for these protein fibrils as efficient carriers for iron fortification. We use biodegradable amyloid fibrils from β-lactoglobulin, an inexpensive milk protein with natural reducing effects, as anti-oxidizing nanocarriers and colloidal stabilizers for iron nanoparticles. The resulting hybrid material forms a stable protein-iron colloidal dispersion that undergoes rapid dissolution and releases iron ions during acidic and enzymatic in vitro digestion. Importantly, this hybrid shows high in vivo iron bioavailability, equivalent to ferrous sulfate in haemoglobin-repletion and stable-isotope studies in rats, but with reduced organoleptic changes in foods. Feeding the rats with these hybrid materials did not result in abnormal iron accumulation in any organs, or changes in whole blood glutathione concentrations, inferring their primary safety. Therefore, these iron-amyloid fibril hybrids emerge as novel, highly effective delivery systems for iron in both solid and liquid matrices.

Formation of Colloidal Nanocellulose Glasses and Gels

Nanocellulose (NC) suspensions can form rigid volume-spanning arrested states (VASs) at very low volume fractions. The transition from a free-flowing dispersion to a VAS can be the result of either an increase in particle concentration or a reduction in interparticle repulsion. In this work, the concentration-induced transition has been studied with a special focus on the influence of the particle aspect ratio and surface charge density, and an attempt is made to classify these VASs. The results show that for these types of systems two general states can be identified: glasses and gels. These NC suspensions had threshold concentrations inversely proportional to the particle aspect ratio. This dependence indicates that the main reason for the transition is a mobility constraint that, together with the reversibility of the transition, classifies the VASs as colloidal glasses. If the interparticle repulsion is reduced, then the glasses can transform into gels. Thus, depending on the preparation route, either soft and reversible glasses or stiff and irreversible gels can be formed.

Biopolymer Aerogels and Foams: Chemistry, Properties, and Applications

Biopolymer aerogels were among the first aerogels produced, but only in the last decade has research on biopolymer and biopolymer-composite aerogels become popular, motivated by sustainability arguments, their unique and tunable properties, and ease of functionalization. Biopolymer aerogels and open-cell foams have great potential for classical aerogel applications such as thermal insulation, as well as emerging applications in filtration, oil-water separation, CO2 capture, catalysis, and medicine. The biopolymer aerogel field today is driven forward by empirical materials discovery at the laboratory scale, but requires a firmer theoretical basis and pilot studies to close the gap to market. This Review includes a database with over 3800 biopolymer aerogel properties, evaluates the state of the biopolymer aerogel field, and critically discusses the scientific, technological, and commercial barriers to the commercialization of these exciting materials.

Ice-Templated and Cross-Linked Amyloid Fibril Aerogel Scaffolds for Cell Growth

Amyloid fibrils prepared from β-lactoglobulin were used to form freeze-dried and cross-linked aerogels. By varying the fibril concentration and freezing gradient, it was possible to control the pore structure and elastic modulus of the aerogels within one order of magnitude from ∼20 to ∼200 kPa. Using butane tetracarboxylic acid as cross-linker, these aerogels maintained their monolithic shape under aqueous conditions, displaying elastic behavior and a modulus in the range of ∼4-40 kPa. When explored as scaffolds for cell growth, the amyloid fibril aerogels demonstrated biocompatibility and led to the successful penetration and permeation of two epithelial cell lines (Caco-2 and HT29) throughout the scaffold. These soft, elastic, and water-stable biomaterials expand the scope of amyloid fibril aerogels, making them suitable for wet-state applications such as heterogeneous catalysis, purification membranes, and 3D matrices for cell growth.

Confinement-induced liquid crystalline transitions in amyloid fibril cholesteric tactoids

Chirality is ubiquitous in nature and plays crucial roles in biology, medicine, physics and materials science. Understanding and controlling chirality is therefore an important research challenge with broad implications. Unlike other chiral colloids, such as nanocellulose or filamentous viruses, amyloid fibrils form nematic phases but appear to miss their twisted form, the cholesteric or chiral nematic phases, despite a well-defined chirality at the single fibril level. Here we report the discovery of cholesteric phases in amyloids, using β-lactoglobulin fibrils shortened by shear stresses. The physical behaviour of these new cholesteric materials exhibits unprecedented structural complexity, with confinement-driven ordering transitions between at least three types of nematic and cholesteric tactoids. We use energy functional theory to rationalize these results and observe a chirality inversion from the left-handed amyloids to right-handed cholesteric droplets. These findings deepen our understanding of cholesteric phases, advancing their use in soft nanotechnology, nanomaterial templating and self-assembly.Left-handed amyloid fibrils form nematic and right-handed cholesteric tactoids with confinement-induced transitions from an ordered to an ordered state.