Controlling the optical properties of chiral nematic mesoporous organosilica films with bioadditives.

Chiral nematic mesoporous organosilica (CNMO) films have unique iridescent properties that make them attractive candidates for decorations, sensing and photonics. However, it has proven difficult to control the colour and porosity of CNMO films. Here, we have explored the addition of a range of biodegradable and eco-friendly additives to tune the helical pitch and, hence, the colour of the CNMO materials.

Cathodic electrodeposition of organic nanocomposite coatings reinforced with cellulose nanocrystals.

A systematic examination of the structure-property relations to create nanocomposite coatings electrophoretic deposition (EPD) of a cathodic polymer - for instance, polyacrylate - reinforced with cellulose nanocrystals (CNCs) is discussed in this work. EPD, a scalable and green technique, has also been used in our approach to polymerize dopamine in the presence of CNCs and cathodic polymer to improve adhesion properties. This study investigated the interactions between CNCs, polydopamine (PDA) and the cathodic polyacrylic polymer to elucidate the dispersion state of the nanoparticles in the system by carefully examining -potential, particle size, and electrophoretic mobility dependence in the colloidal suspension.

Self-assembly of cellulose nanocrystals confined to square capillaries.

Biological systems exploit restricted degrees of freedom to drive self-assembly of nano- and microarchitectures. Simplified systems, such as colloidal nanoparticles that behave as lyotropic liquid crystalline mesophases in confined geometric spaces, may be used to mimic biological structures. Cellulose nanocrystals (CNCs) are colloidally stable nanoparticles that self-assemble into chiral nematic () liquid crystalline mesophases.

Halloysite nanotubes enhance the mechanical properties and thermal stability of iridescent cellulose nanocrystal films.

Films of cellulose nanocrystals (CNCs) with chiral nematic organization can show vivid iridescence that arises from their hierarchical structure. Unfortunately, the brittleness of the films limits their potential applications. In this paper, we investigate the incorporation of halloysite nanotubes (HNTs) into CNC films to prepare organic-inorganic composite films with enhanced mechanical properties, while preserving the chiral nematic structure and brilliant iridescence.

Mechanically Responsive Circularly Polarized Luminescence from Cellulose-Nanocrystal-Based Shape-Memory Polymers.

Stimulus-responsive materials that display circularly polarized luminescence (CPL) have attracted great attention for application in chiral sensors and smart displays. However, due to difficulties in the regulation of chiral structures, fine control of CPL remains a challenge. Here, it is demonstrated that cellulose nanocrystal shape-memory polymers (CNC-SMPs) with luminescent components enable mechanically responsive CPL.

Coassembly of Cellulose Nanocrystals and Neutral Polymers in Iridescent Chiral Nematic Films.

Photonic materials based on composite films of cellulose nanocrystals (CNCs) and polymers are promising as they can be renewable and show tunable optical and mechanical properties. However, the influence of polymers on CNC self-assembly is not always well understood, and conflicting results are present in the literature. In this study, we incorporate three neutral, water-soluble polymers-poly(ethylene glycol) (PEG), poly(vinyl pyrrolidone) (PVP), and poly(acrylic acid) (PAA)-with different molecular weights into CNC suspensions at various concentrations prior to obtaining iridescent composite thin films by solvent evaporation.

Cellulose Nanocrystal Gels with Tunable Mechanical Properties from Hybrid Thermal Strategies.

Gels are useful materials for drug delivery, wound dressings, tissue engineering, and 3D printing. These various applications require gels with different mechanical properties that can be easily tuned, also preferably excluding the use of chemical additives, which can be toxic or harmful to the body or environment. Here, we report a novel strategy to synthesize cellulose nanocrystal (CNC) gels with tunable mechanical properties.

Concentric chiral nematic polymeric fibers from cellulose nanocrystals.

Hierarchical biological materials, such as osteons and plant cell walls, are complex structures that are difficult to mimic. Here, we combine liquid crystal systems and polymerization techniques within confined systems to develop complex structures. A single-domain concentric chiral nematic polymeric fiber was obtained by confining cellulose nanocrystals (CNCs) and hydroxyethyl acrylate inside a capillary tube followed by UV-initiated polymerization.

How hydrogen-bonding interactions and nanocrystal aspect ratios influence the morphology and mechanical performance of polymer nanocomposites reinforced with cellulose nanocrystals.

The performance of polymer nanocomposites reinforced with cellulose nanocrystals (CNCs) is complicated by several factors, primarily CNC-polymer and polymer-polymer interactions. Our current work specifically seeks to address the effects of CNC geometry, CNC-polymer and polymer-polymer interactions on the structure and non-linear mechanical performance of nanocomposites prepared using two water-soluble polymers, polyethylene oxide (PEO) and polyvinyl alcohol (PVA), having different morphological and structural characteristics. PEO and PVA are chosen since they are compatible with CNCs, however, they interact quite differently with CNCs and result in different reinforcement mechanisms.

Using rotation to organize cellulose nanocrystals inside a fiber.

We demonstrate for the first time that continuous rotation of a mixture of cellulose nanocrystals (CNCs) and monomer in a capillary tube results in well-organized structures. In the experiments, a capillary tube charged with an aqueous suspension of CNCs and hydroxyethyl acrylate was continuously rotated, then the structure was fixed in place by UV-initiated polymerization. The organization of the liquid crystalline structure that forms inside the tube depends on the rotation conditions and is captured in the polymer resin.

Fast Self-Assembly of Scalable Photonic Cellulose Nanocrystals and Hybrid Films via Electrophoresis.

Nano-enabled, bio-based, functional materials are key for the transition to a sustainable society as they can be used, owing to both their performance and nontoxicity, to gradually replace existing nonrenewable engineering materials. Cellulose nanocrystals (CNCs), produced by acid hydrolysis of cellulosic biomass, have been shown to possess distinct self-assembly, optical, and electromechanical properties, and are anticipated to play an important role in the fabrication of photonic, optoelectronic, and functional hybrid materials. To facilitate CNCs' technological viability, a method suitable for industrial exploitation is developed to produce photonic films possessing long-range chirality on conductive, rigid, or flexible, substrates within a few minutes.

A rheological investigation of oil-in-water Pickering emulsions stabilized by cellulose nanocrystals.

Hypothesis: High and medium internal phase Pickering emulsions stabilized with cellulose nanocrystals (CNCs) exhibited very different performance compared to their peers stabilized with a surfactant. In this paper, we ascribed the difference to the formation of hydrogen bonding and van der Waals interactions between the CNC nanoparticles on adjacent oil droplets.

Experiments: Rheological properties of CNC-stabilized oil-in-water medium internal phase emulsions (MIPEs, oil content = 65% v/v) and high internal phase emulsions (HIPEs, oil content = 80% v/v) were comprehensively characterized using both oscillatory and rotational tests.

Effect of thermal treatments on chiral nematic cellulose nanocrystal films.

The ability to manipulate the optical appearance of materials is essential in virtually all products and areas of technology. Structurally coloured chiral nematic cellulose nanocrystal (CNC) films proved to be an excellent platform to design optical appearance, as their response can be moulded by organising them in hierarchical architectures. Here, we study how thermal treatments influence the optical appearance of structurally coloured CNC films.

Properties and stabilization mechanism of oil-in-water Pickering emulsions stabilized by cellulose filaments.

Cellulose filaments (CFs) are produced from wood-pulp fibres through solely mechanical treatment. They are inhomogeneous materials comprising both relatively large fibre fragments and fine fibrils. CFs can stabilize oil-in-water medium- and high-internal phase Pickering emulsions, where the presence of fibre fragments plays a critical role in emulsion stabilization by preventing CF fibrils from forming highly entangled structures.

Thermal Degradation of Cellulose Filaments and Nanocrystals.

Cellulose-derived materials, such as microcellulose and nanocellulose, are sustainable materials with a wide range of applications. Here, through a multi-analytical approach, we investigate the thermal degradation of microfibrillar cellulose filaments (CFs); acidic cellulose nanocrystals (CNC-H), containing sulfate half-ester groups on the surface; and neutralized cellulose nanocrystals (CNC-Na), where the protons are replaced by sodium ions. CFs have a simple degradation mechanism, associated with extensive dehydration, decarboxylation, and decarbonylation, and the highest thermal stability of the three (∼325 °C) despite the abundance of amorphous regions and inhomogeneous fibrous mass that make them structurally and morphologically less homogeneous than high-crystallinity CNCs.

Retrieving the Coassembly Pathway of Composite Cellulose Nanocrystal Photonic Films from their Angular Optical Response.

Aqueous suspensions of cellulose nanocrystals (CNCs) are known to self-assemble into a chiral nematic liquid crystalline phase, leading to solid-state nanostructured colored films upon solvent evaporation, even in the presence of templating agents. The angular optical response of these structures, and therefore their visual appearance, are completely determined by the spatial arrangement of the CNCs when the drying suspension undergoes a transition from a flowing and liquid crystalline state to a kinetically arrested state. Here, it is demonstrated how the angular response of the final film allows for retrieval of key physical properties and the chemical composition of the suspension at the onset of the kinetic arrest, thus capturing a snapshot of the past.

Tunable Diffraction Gratings from Biosourced Lyotropic Liquid Crystals.

Diffraction gratings are important for modern optical components, such as optical multiplexers and signal processors. Although liquid crystal (LC) gratings based on thermotropic LCs have been extensively explored, they often require expensive molecules and complicated manufacturing processes. Lyotropic LCs, which can be broadly obtained from both synthetic and natural sources, have not yet been applied in optical gratings.

Improving Thin-Film Properties of Poly(vinyl alcohol) by the Addition of Low-Weight Percentages of Cellulose Nanocrystals.

The increased demand for electronic devices, combined with a desire to minimize the environmental impact, necessitates the development of new eco-friendly materials. One promising approach is the incorporation of renewable and green materials that possess the desired mechanical and electrical properties while allowing for more ecologically friendly disposal of these devices. The addition of low-weight percentages (0.

Iridescent Cellulose Nanocrystal Films Modified with Hydroxypropyl Cellulose.

The introduction of polymers into a chiral nematic cellulose nanocrystal (CNC) matrix allows for the tuning of optical and mechanical properties, enabling the development of responsive photonic materials. In this study, we explored the incorporation of hydroxypropyl cellulose (HPC) into a CNC film prepared by slow evaporation. In the composite CNC/HPC thin films, the CNCs adopt a chiral nematic structure, which can selectively reflect certain wavelengths of light to yield a colored film.

Host-Guest Chemistry Within Cellulose Nanocrystal Gel Receptors.

Cellulose nanocrystals (CNCs) spontaneously assemble into gels when mixed with a polyionic organic or inorganic salt. Here, we have used this ion-induced gelation strategy to create functional CNC gels with a rigid tetracationic macrocycle, cyclobis(paraquat-p-phenylene) (CBPQT ). Addition of [CBPQT]Cl to CNCs causes gelation and embeds an active host inside the material.

Microsuspension Polymerization of Styrene Using Cellulose Nanocrystals as Pickering Emulsifiers: On the Evolution of Latex Particles.

We report a mechanistic study of the microsuspension polymerization of styrene stabilized by cellulose nanocrystals (CNCs) in its native form as well as graft-modified with copolymers of styrene and -3-(dimethylamino)propyl methacrylamide (DMAPMAm) or ,-(diethylamino)ethyl methacrylate (DEAEMA). Native CNCs and graft-modified CNCs were shown to form stable styrene emulsions with an average droplet diameter of 18-20 and 5-9 μm, respectively. Initiators of widely varying water solubilities [2,2'-azobisisobutyronitrile (AIBN), 2-2'-azobis(2,4-dimethylvaleronitrile) (Vazo-52), and lauroyl peroxide (LPO)] were employed for the polymerizations.

Cellulose Nanocrystal Elastomers with Reversible Visible Color.

Responsive photonic crystals have potential applications in mechanical sensors and soft displays; however, new materials are constantly desired to provide new innovations and improve on existing technologies. To address this, we report stretchable chiral nematic cellulose nanocrystal (CNC) elastomer composites that exhibit reversible visible color upon the application of mechanical stress. When stretched (or compressed) the colorless materials maintain their chiral nematic structure but the helical pitch is reduced into the visible region, resulting in coloration of the CNC-elastomer composite.

Post-modification of Cellulose Nanocrystal Aerogels with Thiol-Ene Click Chemistry.

The functionalization of cellulose nanocrystal (CNC) aerogels was achieved through a two-step synthetic procedure. CNC aerogels were prepared under hydrothermal conditions, followed by solvent exchange and critical point drying. The CNC aerogels were functionalized with a methacrylate group and then underwent thiol-ene click chemistry to impart a range of functionalities onto the surface of the CNC aerogel.

Freeze-Thaw Gelation of Cellulose Nanocrystals.

Gels are attractive for applications in drug delivery, tissue engineering, and 3D printing. Here, physical colloidal gels were prepared by freeze-thaw (FT) cycling of cellulose nanocrystal (CNC) suspensions. The aggregation of CNCs was driven by the physical confinement of CNCs between growing ice crystal domains.