Moisture-driven energy generators (MEGs) utilizing cellulose, which are renowned for their inherent eco-friendliness, have garnered considerable attention; however, their stability, recyclability, and high performance remain to be demonstrated. Specifically, compromised structural integrity, particularly under moist conditions, severely curtails their long-term operational viability. We developed a highly stable cellulose MEG that operated continuously for 350 h with a maintained open circuit voltage of 0.703 V. The enhancement of cellulose MEG performance was achieved via a robust structural framework realized through a composite of cellulose nanofibers (CNFs) cross-linked with citric acid, alongside electrically conductive carbon nanotubes (CNTs). We engineered a free-standing bilayer-type cellulose MEG featuring a chemically networked CNF/CNT composite onto a moisture-supplying ionic organohydrogel. Our crosslinked cellulose MEG achieved a short-circuit current density of 39 μA cm⁻² and a maximum power density of 28.9 μW cm⁻². Moreover, the crosslinked CNF/CNT aerogel was successfully biodegraded with an enzyme after energy generation. The recycled cellulose MEG, utilizing recovered CNTs and reused ionic organohydrogel, achieved an impressive output of 98.8% compared with that of the original MEG. Our MEG finds practical utility as a temperature sensor in smart packaging for continuous monitoring. Our crosslinked cellulose MEG achieves sustainability via recyclability and enhancing its practical applicability.

Cellulose nanofibrils (CNFs) have attracted much attention because of their renewability and potential biocompatibility. However, CNFs are extremely hydrophilic due to the presence of a large number of hydroxyl groups, limiting their use as a water-resistant material. In this work, we controlled the adsorption behavior of silica nanoparticles on the surface of CNFs by adjusting the synthesis conditions. The silica nanoparticle size and packing efficiency on the CNF surface could be controlled by varying the ammonium hydroxide and water concentrations. In addition, hexadecyltrimethoxysilane (HDTMS) was successfully grafted onto CNF or CNF/silica nanocomposite surfaces, and the quantitative content of organic/inorganic substances in HDTMS was analyzed through XPS and TGA. The HDTMS-modified CNF/silica nanocomposites were more advantageous in terms of hydrophobicity than the HDTMS-modified CNF composites. This is because the silica nanoparticles were adsorbed on the surface of the CNFs, increasing the surface roughness and simultaneously increasing the amount of HDTMS. As a result, the HDTMS-modified CNFs showed a water contact angle (WCA) of ~80°, whereas HDTMS-modified CNF/silica nanocomposites obtained superhydrophobicity, with a WCA of up to ~159°. This study can provide a reference for the expansion of recyclable eco-friendly coating materials via the adsorption of silica nanoparticles and hydrophobic modification of CNF materials.

The design and fabrication of oxygen barrier films is important for both fundamental and industrial applications. We prepared three different thin films composed of graphene oxide (GO) and laponite (LN), a typical low cost inorganic clay, with the GO/LN volume ratios of 1.9/0.1, 1.7/0.3 and 1.5/0.5 together with a double layer film of the GO and LN. We found that the films with GO/LN = 1.9/0.1 and the double layers exhibited high oxygen barrier and oxygen transmission rate values that reached 0.55 and 0.37 cm³ per m² per atm per day, respectively, which were much lower than those of the films prepared from the pure GO, only LN and GO/LN = 1.7/0.3 and 1.5/0.5. This study is important for the design and fabrication of a film from GO-based all inorganic nanomaterials for applications in gas-barrier membranes.

Since the plastic-based multilayer films applied to food packaging are not recyclable, it is necessary to develop easily recyclable single materials. Herein, polypropylene (PP)-based cellulose nanofiber (CNF)/nanoclay nanocomposites were prepared by melt-mixing using a fixed CNF content of 1 wt %, while the nanoclay content varied from 1 to 5 wt %. The optimum nanoclay content in the PP matrix was found to be 3 wt % (PCN3), while they exhibited synergistic effects as a nucleating agent. PCN3 exhibited the best mechanical properties, and the tensile and flexural moduli were improved by 51% and 26%, respectively, compared to PP. In addition, the oxygen permeability was reduced by 28%, while maintaining the excellent water vapor permeability of PP. The improvement in the mechanical and barrier properties of PP through the production of PP/CNF/nanoclay hybrid nanocomposites suggested their possible application in the field of food packaging.