Reconstruction of Cellulose Intermolecular Interactions from Hydrogen Bonds to Dynamic Covalent Networks Enables a Thermo-processable Cellulosic Plastic with Tunable Strength and Toughness

Abstract

Its excellent renewability and biodegradability make cellulose an attractive resource to prepare fossil-based plastic alternatives. However, cellulose itself exhibits strong intermolecular hydrogen bond (H-bond) interactions, significantly restricting the mobility of cellulose chains, thus leading to poor thermo-processing performance. Here, we reconstructed the intermolecular interactions of cellulose chains via replacing the original H-bonds with dynamic covalent bonds. By this, cellulose can be easily thermo-processed into a cellulosic plastic under mild conditions (70 °C). Through adjusting the chemical structure of dynamic covalent networks, the cellulosic plastic shows tunable mechanical strength (3.0–33.5 MPa) and toughness (43–321 kJ m–2). The cellulosic plastic also exhibits excellent resistance to water, organic solvent, acid solution, alkali solution, and high temperature (>400 °C). Moreover, it owns good chemical and biological degradability and recyclability. This work provides an effective method to develop high-performance cellulosic plastics for fossil-based plastic substitution.

Insight into the Feasibility of Fatty Acyl Chlorides with 10–18 Carbons for the Ball-Milling Synthesis of Thermoplastic Cellulose Esters

“…Current sustainable development urged the imperative exploration and utilization of renewable resources. − Among numerous renewable resources, cellulose is the most abundant and has infinite potential for exploiting eco-friendly polymer materials to relieve plastic pollution and resource scarcity. − However, strong hydrogen-bond networks caused by chain stereoregularity and abundant hydroxyl (−OH) groups lead to the poor processability (including solubility and thermoplasticity) of cellulose. − In other words, feasibly shaping cellulose into high-value products remains challenging.…”

Enhancing Aging Resistance of Transparent Paper: Structural Modification of Wood Fibers via Carboxymethylation

“…Based on the different treatments of fiber raw materials, the papermaking method can be further classified into direct mechanical treatment, chemical modification approaches, etc . Among these, chemical modification of wood fibers has proven to be a practical and cost-effective method with broad applicability. , By introducing anionic groups to the fiber surface, chemical modification increases electrostatic repulsion, causing fibers to swell, changing their morphology, and resulting in a tighter bond within the paper, thereby enhancing its transparency. ,− Commonly employed chemical modification methods include TEMPO oxidation, sulfated, etc. − Fang and colleagues have created highly transparent paper by chemically modifying wood fibers with TEMPO oxidation, achieving approximately 90% light transmittance and 60% haze at 550 nm . Recent advancements have further improved these papers, with light transmission and haze reaching above 90 and 80%, respectively …”

Preparation and evaluation of bioactive cellulose acetate films from Musa acuminata

“…3 As the most abundant renewable and biodegradable biopolymer, cellulose is seen to be one of the most promising substitutes for plastic. 4 While cellulose holds promise as a renewable and biodegradable alternative to fossil-based plastics, its thermo-processing performance is hindered by the presence of robust intermolecular hydrogen bond interactions. These interactions limit chain mobility, thereby posing challenges to the efficient conversion of cellulose into plastic materials.…”