This review summarizes the preparation methods of cellulose nanofibrils (CNFs) and the progress in the research pertaining to their surface modification. Moreover, the preparation and surface modification of nanocellulose were comprehensively introduced based on the existing literature. The review focuses on the mechanical treatment of cellulose, the surface modification of fibrillated fibers during pretreatment, the surface modification of nanocellulose and the modification of CNFs and their functional application. In the past five years, research on cellulose nanofibrils has progressed with developments in nanomaterials research technology. The number of papers on nanocellulose alone has increased by six times. However, owing to its high energy consumption, high cost and challenging industrial production, the applications of nanocellulose remain limited. In addition, although nanofibrils exhibit strong biocompatibility and barrier and mechanical properties, their high hydrophilicity limits their practical application. Current research on cellulose nanofibrils has mainly focused on the industrial production of CNFs, their pretreatment and functional modification and their compatibility with other biomass materials. In the future, with the rapid development of modern science and technology, the demand for biodegradable biomass materials will continue to increase. Furthermore, research on bio-based nanomaterials is expected to advance in the direction of functionalization and popularization.

Because of its non-toxic, pollution-free, and low-cost advantages, environmentally-friendly packaging is receiving widespread attention. However, using simple technology to prepare environmentally-friendly packaging with excellent comprehensive performance is a difficult problem faced by the world. This paper reports a very simple and environmentally-friendly method. The hydroxyl groups of cellulose nanofibrils (CNFs) were modified by introducing malic acid and the silane coupling agent KH-550, and the modified CNF were added to cassava starch as a reinforcing agent to prepare film with excellent mechanical, hydrophobic, and barrier properties. In addition, due to the addition of malic acid and a silane coupling agent, the dispersibility and thermal stability of the modified CNFs became significantly better. By adjusting the order of adding the modifiers, the hydrophobicity of the CNFs and thermal stability were increased by 53.5% and 36.9% ± 2.7%, respectively. At the same time, the addition of modified CNFs increased the tensile strength, hydrophobicity, and water vapor transmission coefficient of the starch-based composite films by 1034%, 129.4%, and 35.95%, respectively. This material can be widely used in the packaging of food, cosmetics, pharmaceuticals, and medical consumables.

Composite films of polybutylene adipate terephthalate (PBAT) were prepared by adding thermoplastic starch (TPS) (TPS/PBAT) and nano-zinc oxide (nano-ZnO) (TPS/PBAT/nano-ZnO). The changes of surface morphology, thermal properties, crystal types and functional groups of starch during plasticization were analyzed by scanning electron microscopy, synchronous thermal analysis, X-ray diffraction, infrared spectrometry, mechanical property tests, and contact Angle and transmittance tests. The relationship between the addition of TPS and the tensile strength, transmittance, contact angle, water absorption, and water vapor barrier of the composite film, and the influence of nano-ZnO on the mechanical properties and contact angle of the 10% TPS/PBAT composite film. Experimental results show that, after plasticizing, the crystalline form of starch changed from A-type to V-type, the functional group changed and the lipophilicity increased; the increase of TPS content, the light transmittance and mechanical properties of the composite membrane decreased, while the water vapor transmittance and water absorption increased. The mechanical properties of the composite can be significantly improved by adding nano-ZnO at a lower concentration (optimum content is 1 wt%).

Cost-effective, practical, and efficiently performing photosensitive resin composite materials are essential, as the current materials are expensive, lack better alternatives, and do not meet 3D printing standards. In this study, based on orthogonal experiments for photosensitive resin curing, we prepared a free-radical/cationic hybrid photosensitive UV cured resin (UVR) using acrylic ester and epoxy resin as the prepolymers, tripropylenediol diacrylate (TPGDA) as the active diluent, and triaryl sulfonium salt (I-160) and 2,2-dimethyl-α-hydroxy acetophenone (1173) as the photoinitiators, in the optimized formula of acrylic-ester:epoxy-resin:TPGDA:I-160:1173 = 37.5:37.5:20:2.5:2.5. Further, we investigated the effects of polyurethane acrylates (PUA) and Graphene oxide (GO) on the surface morphology, chemical structure, hydrophobicity, mechanical strength, and gelation rate of the hybrid resin. We observed that 20% PUA improved tensile strength to the maximum of 36.89 MPa from 16.42 MPa of the unmodified hybrid resin, whereas 1% GO reduced volume shrinkage to the minimum of 2.89% from 3.73% of the unmodified hybrid resin. These photosensitive resins with higher tensile strength and lower volume shrinkage can be used to synthesize high performance functional materials in the future.

In this study, we investigated the barrier properties of a montmorillonite-reinforced biomass material, starch. Organically modified montmorillonite materials were prepared from natural montmorillonite by reacting it with dodecyl trimethyl ammonium chloride, dodecyl dimethyl benzyl ammonium chloride or octadecyl trimethyl ammonium chloride under ultrasonic conditions. The composite starch films incorporated with these organically modified montmorillonite samples were characterized by scanning electron microscopy, transmission electron microscopy, infrared spectroscopy and X-ray diffraction. The results showed that the introduction of montmorillonite decreases the transmittance of the composite film by 10% in the visible region and significantly inhibits UV-light transmittance. The decomposition temperature of the composite film ranges from 200 to 500 °C, with a weight loss rate of 80%. The distance between the montmorillonite layers increases from 0.14 nm in the non-magnetized state to 1.49 nm after magnetization. The oxygen permeability of the starch film modified by organic montmorillonite (0.067 cm³/m²·d) is lower than that of the montmorillonite starch film without magnetization (0.097cm³/m²·d). The oxygen barrier capacity is close to zero. Particularly in the ordered magnetic montmorillonite starch composite film, the oxygen barrier ability is the best. Therefore, modified montmorillonite could serve as an excellent reinforcing agent for cassava starch films and effectively improve the oxygen barrier performance of the films.

Polylactic acid (PLA) is extensively used as a raw material in fused deposition modeling (FDM)-based three-dimensional printing (3DP), owing to its abundant resources, simple production processes, decent biodegradability, and adequate mechanical strength. However, it has disadvantages such as poor toughness and straightforward bending deformation. Given the considerable application potential of PLA materials in FDM-based 3DP technology, herein, studies conducted over the last 5 years toward the enhancement of the characteristics of PLA for FDM are summarized. In particular, modification approaches (chemical or physical methods) that have been employed to improve the mechanical and processing attributes of PLA are discussed, along with the development of PLA composites with unique functionalities. The insights provided herein can help expand the scope of application of PLA composites in FDM-based 3DP for utilization in fields such as transportation, aerospace engineering, industrial equipment fabrication, consumer/electronic product manufacturing, and biomedicine/medicine.