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. The color could be tuned across the visible spectrum by changing the concentration or molecular weight of the HPC. Importantly, the composite films were more flexible than pure CNC films with up to a ten-fold increase in elasticity and a decrease in stiffness and tensile strength of up to six times and four times, respectively. Surface modification of the films with methacrylate groups increased the hydrophobicity of the films, and therefore, the water stability of these materials was also improved.
Mineral dust particles are one of the most abundant types of ice nucleating particles in the atmosphere. During atmospheric transport, these particles can be coated with water-soluble solutes, which can modify their ice nucleating ability. Although previous studies have shown that even low concentrations of water-soluble solutes can modify the ice nucleating properties of mineral dust particles, our understanding of this topic is far from complete. We examined the effects of a series of alkali metal nitrates at low concentrations (5 × 10 −5 M to 5 × 10 −3 M) on the surface composition and immersion freezing of potassium-rich feldspar (K-rich feldspar). Immersion freezing was investigated with the droplet freezing technique, and the surface composition was investigated with cryogenic X-ray photoelectron spectroscopy. K + increased the median freezing temperature of the droplets, while the other alkali metal cations either had no effect or decreased the median freezing temperature. The changes in the median freezing temperature of the droplets due to the presence of nitrates followed the order K + ≥ Li + ≥ Na + ≥ Rb + ≥ Cs + and, except for Cs + , were correlated to the K/Al ratio at the surface of K-rich feldspar. The K/Al ratio is possibly an indicator of the abundance of certain types of K-bearing microcline surfaces that drive the immersion freezing of K-rich feldspar, while Cs + likely influences the immersion freezing of K-rich feldspar by an additional mechanism, possibly blocking ice nucleation sites by adsorption. Our work also shows that the cation charge density (charge density over the surface area of a single cation) is not a good predictor of the effects of cations on the immersion freezing of K-rich feldspar in our experiments.
The development of novel aerogel materials with chiral nematic ordered structures offers exciting pathways for the fabrication of multifunctional hybrid materials with enhanced functionality. Aerogels prepared from cellulose nanocrystals are especially interesting due to their unique structural properties. To promote applicability in energy storage materials, it is often necessary to incorporate metals and metal oxides into three-dimensional porous nanostructures. In this study, germania was incorporated into a chiral nematic cellulose nanocrystal aerogel using a sol–gel method. Interestingly, our approach does not disturb the order of the original chiral nematic CNC aerogels, providing hybrid aerogels with a large concentration of randomly distributed GeO2 nanoparticles and specific surface areas up to 705 m2 g–1. Carbonization of the composite material afforded a highly ordered material with no collapse during compression and good shape recovery after release. The combination of the electrochemical double layer capacitance provided by the carbonaceous skeleton and the pseudocapacitive contribution from the GeO2 nanoparticles resulted in materials with a maximum C p of 113 F g–1 that exhibited good capacitance retention. To push the boundaries of safer energy storage devices based on renewable resources, we demonstrate the preparation of an all-cellulose solid-state symmetric supercapacitor.
Plexitonic nanoparticles offer variable optical properties through tunable excitations, in addition to electric field enhancements that far exceed molecular resonators. This study demonstrates a way to design an ultrabright surface-enhanced Raman spectroscopy (SERS) signal while simultaneously quenching the fluorescence background through silica encapsulation of the semiconductor-metal composite nanoparticles. Using a multistep approach, a J-aggregate-forming organic dye is assembled on the surface of gold nanoparticles using a cationic linker. Excitonic resonance of the J-aggregate-metal system shows an enhanced SERS signal at an appropriate excitation wavelength. Further encapsulation of the decorated particles in silica shows a significant reduction in the fluorescence signal of the Raman spectra (5× reduction) and an increase in Raman scattering (7× enhancement) when compared to phospholipid encapsulation. This reduction in fluorescence is important for maximizing the useful SERS enhancement from the particle, which shows a signal increase on the order of 10 times greater than J-aggregated dye in solution and 24 times greater than Oxonica S421 SERS tag. The silica layer also serves to promote colloidal stability. The combination of reduced fluorescence background, enhanced SERS intensity, and temporal stability makes these particles highly distinguishable with potential to enable high-throughput applications such as SERS flow cytometry.
A cellulose nanocrystal liquid crystalline suspension was mixed with monomers and confined to a capillary tube. After photopolymerization, a fiber with a single-domain concentric chiral nematic structure throughout the length of the fiber was obtained.
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