Processing factors affecting roughness, optical and mechanical properties of nanocellulose films for optoelectronics.

This work aims to understand how nanocellulose (NC) processing can modify the key characteristics of NC films to align with the main requirements for high-performance optoelectronics. The performance of these devices relies heavily on the light transmittance of the substrate, which serves as a mechanical support and optimizes light interactions with the photoactive component. Critical variables that determine the optical and mechanical properties of the films include the morphology of cellulose nanofibrils (CNF), as well as the concentration and turbidity of the respective aqueous suspensions. This study demonstrates that achieving high transparency was possible by reducing the grammage and adjusting the drying temperature through hot pressing. Furthermore, the use of modified CNF, specifically carboxylated CNF, resulted in more transparent films due to a higher nanosized fraction and lower turbidity. The mechanical properties of the films depended on their structure, homogeneity (spatial uniformity of local grammage), and electrokinetic factors, such as the presence of electrostatic charges on CNF. Additionally, we investigated the angle-dependent transmittance of the CNF films, since solar devices usually operate under indirect light. This work demonstrates the importance of a systematic approach to the optimization of cellulose films, providing valuable insight into the optoelectronic field.

Design of experiments to investigate multi-additive cellulose nanocrystal films.

Cellulose nanocrystal (CNC) suspensions can self-assemble into chiral nematic films upon the slow evaporation of water. These films are brittle, as indicated by their fracturing instead of plastically deforming once they are fully elastically deformed. This aspect can be mediated to some extent by plasticizing additives, such as glucose and glycerol, however, few reports consider more than one additive at a time or address the influence of additive content on the homogeneity of the self-assembled structure. In this work, design of experiments (DoE) was used to empirically model complex film compositions, attempting to relate additive concentrations in dilute suspension to film properties, and to understand whether outcome specific predictions are possible using this approach. We demonstrate that DoE can be used to predict film properties in multi-additive systems, without consideration given to the different phenomena that occur along the drying process or to the nature of the additives. Additionally, a homogeneity metric is introduced in relation to chiral nematic organization in CNC films, with most of the additive-containing compositions in this work found to reduce the homogeneity of the self-assembly relative to pure CNC films.

Perspective about Cellulose-Based Pressure and Strain Sensors for Human Motion Detection.

High-performance wearable sensors, especially resistive pressure and strain sensors, have shown to be promising approaches for the next generation of health monitoring. Besides being skin-friendly and biocompatible, the required features for such types of sensors are lightweight, flexible, and stretchable. Cellulose-based materials in their different forms, such as air-porous materials and hydrogels, can have advantageous properties to these sensors. For example, cellulosic sensors can present superior mechanical properties which lead to improved sensor performance. Here, recent advances in cellulose-based pressure and strain sensors for human motion detection are reviewed. The methodologies and materials for obtaining such devices and the highlights of pressure and strain sensor features are also described. Finally, the feasibility and the prospects of the field are discussed.

Plant-Based Structures as an Opportunity to Engineer Optical Functions in Next-Generation Light Management.

This review addresses the reconstruction of structural plant components (cellulose, lignin, and hemicelluloses) into materials displaying advanced optical properties. The strategies to isolate the main building blocks are discussed, and the effects of fibrillation, fibril alignment, densification, self-assembly, surface-patterning, and compositing are presented considering their role in engineering optical performance. Then, key elements that enable lignocellulosic to be translated into materials that present optical functionality, such as transparency, haze, reflectance, UV-blocking, luminescence, and structural colors, are described. Mapping the optical landscape that is accessible from lignocellulosics is shown as an essential step toward their utilization in smart devices. Advanced materials built from sustainable resources, including those obtained from industrial or agricultural side streams, demonstrate enormous promise in optoelectronics due to their potentially lower cost, while meeting or even exceeding current demands in performance. The requirements are summarized for the production and application of plant-based optically functional materials in different smart material applications and the review is concluded with a perspective about this active field of knowledge.

Cross-Linked and Surface-Modified Cellulose Acetate as a Cover Layer for Paper-Based Electrochromic Devices.

We studied the surface and microstructure of cellulose acetate (CA) films to tailor their barrier and mechanical properties for application in electrochromic devices (ECDs). Cross-linking of CA was carried out with pyromellitic dianhydride to enhance the properties relative to unmodified CA: solvent resistance (by 43% in acetone and 37% in DMSO), strength (by 91% for tensile at break), and barrier (by 65% to oxygen and 92% to water vapor). Surface modification via tetraethyl orthosilicate and octyltrichlorosilane endowed the films with hydrophobicity, stiffness, and further enhanced solvent resistance. A detailed comparison of structural, chemical, surface, and thermal properties was performed by using X-ray diffraction, dynamic mechanical analyses, Fourier-transform infrared spectroscopy, and atomic force microscopy. Coplanar ECDs were synthesized by incorporating a hydrogel electrolyte comprising TEMPO-oxidized cellulose nanofibrils and an ionic liquid. When applied as the top layer in the ECDs, cross-linked and hydrophobized CA films extended the functionality of the assembled displays. The results indicate excellent prospects for CA films in achieving environmental-friendly ECDs that can replace poly(ethylene terephthalate)-based counterparts.

Investigating effects of high cellulase concentration on the enzymatic hydrolysis of the sisal cellulosic pulp.

The goal of this study was to investigate how the use of high concentration of cellulase may impact the properties of the substrate and the reaction medium during the enzymatic hydrolysis of the sisal pulp. Enzyme concentration of 0.9 mL g-1 was considered for hydrolysis of a sisal cellulosic substrate, and the results were compared with previous ones using 0.5 mL g-1 as cellulase concentration. Nonhydrolyzed pulps and the liquors were withdrawn from the reaction medium and characterized by scanning electron microscopy, crystallinity index, average molar mass, length/thickness, and high-performance liquid chromatography (HPLC). The results indicated that the enzyme/substrate ratio impacted crystallinity variations during the reaction and the induction period for exoglucanase action. The concentration of 0.9 mL g-1 led to a glucose yield (98%, an almost quantitative conversion) higher than 0.5 mL g-1 (89%). Aiming to gain information on the post-burst phase (after 15 h), 1 g of sisal pulp was added, and the results demonstrated that the enzymes remained active, which can counterbalance the higher cost due to the use of high enzymes concentrations. This study deepened the understanding of the enzymatic hydrolysis of sisal cellulosic pulp, and the findings may also benefit investigations on other pulps.