Despite the significant properties of fossil plastics, the current unsustainable methods employed in production, usage and disposal present a grave threat to both energy and environment. The development of degradable biomass materials as substitutes for fossil plastics can effectively address the energy-environment paradox at the source. Here, we prepared novel micro-nano multiscale composite films through assembling and crosslinking nanocellulose with coniferous wood pulp microfibers. The composite film combines the advantages of microfibers and nanocellulose, achieving a maximum transmittance of 91 %, foldability, excellent mechanical properties (tensile strength: 51.3 MPa, elongation at break: 4 %, young\'s modulus: 3.4 GPa), high thermal stability and complete degradation within 40 days. The composite film exhibits mechanochemical self-healing and retains properties even after fracture. Such exceptional performance fully meets the requirements for substituting petroleum plastics. By incorporating CaAlSiN3:Eu2+ into the composite film, it enables dual emission of red and blue light, thereby being able to promote plant growth and presenting potential as a novel sustainable alternative for agricultural films. By assembling microfiber and nanocellulose, such novel strategy is presented for the fabrication of high-quality biomass materials, thereby offering a promising avenue towards environment-friendly resource-sustainable new materials.

Vat photopolymerization 3D printing has proven very successful for the rapid additive manufacturing (AM) of polymeric parts at high resolution. However, the range of materials that can be printed and their resulting properties remains narrow. Herein, we report the successful AM of a series of poly(carbonate-b-ester-b-carbonate) elastomers, derived from carbon dioxide and bio-derived ϵ-decalactone. By employing a highly active and selective Co(II)Mg(II) polymerization catalyst, an ABA triblock copolymer (Mn=6.3 kg mol-1, ÐM=1.26) was synthesized, formulated into resins which were 3D printed using digital light processing (DLP) and a thiol-ene-based crosslinking system. A series of elastomeric and degradable thermosets were produced, with varying thiol cross-linker length and poly(ethylene glycol) content, to produce complex triply periodic geometries at high resolution. Thermomechanical characterization of the materials reveals printing-induced microphase separation and tunable hydrophilicity. These findings highlight how utilizing DLP can produce sustainable materials from low molar mass polyols quickly and at high resolution. The 3D printing of these functional materials may help to expedite the production of sustainable plastics and elastomers with potential to replace conventional petrochemical-based options.

Piezoelectric nanogenerators (PENGs) are booming for energy collection and wearable energy supply as one of the next generations of green energy-harvesting devices. Balancing the output, safety, degradation, and cost is the key to solving the bottleneck of PENG application. In this regard, yttrium (Y)-doped zinc oxide (ZnO) (Y-ZnO) was synthesized and embedded into polylactide (PLLA) for developing degradable piezoelectric composite films with an enhanced energy-harvesting performance. The synthesized Y-ZnO exhibits high piezoelectric properties benefiting from the stronger polarity of the Y-O bond and regulation of oxygen vacancy concentration, which improve the output performance of the composite film with Y-ZnO and PLLA (Y-Z-PLLA). The obtained open-circuit voltage (Voc), short-circuit current (Isc), and instantaneous power density of the optimized Y-Z-PLLA PENG reach 17.52 V, 2.45 μA, and 1.76 μW/cm2, respectively. The proposed PENG also shows good degradability. In addition, practical applications of the proposed PENG were demonstrated by converting biomechanical energy, such as walking, running, and jumping, into electricity.

Zwitterionic polymers have emerged as an important class of biomaterials to construct wound dressings and antifouling coatings over the past decade due to their excellent hydrophilicity. However, all the reported zwitterionic polymers as wound dressings are nondegradable because of noncleavable carbon─carbon bonding backbones, and must be removed periodically after treatment to avoid hypoxia in the wound, thus leading to potential secondary injury. In this work, a biodegradable polyzwitterion patch is fabricated for the first time by ring-opening polymerization of carboxybetaine dithiolane (CBDS), which is self-crosslinked via inter-amide hydrogen bonds and zwitterionic dipole-dipole interactions on the side chains. The unprecedented polyCBDS (PCBDS) patch demonstrates enough ductility owing to the intermolecular physical interactions to fully cover irregular wounds, also showing excellent biodegradability and antifouling performance resulted from the existence of disulfide bonds and carboxybetaine groups. Besides, the PCBDS degradation-induced released CBDS owns potent antioxidant and antibacterial activities. This PCBDS patch is used as a diabetic wound dressing, inhibiting bacterial adhesion on the external surface, and its degradation products can exactly kill bacteria and scavenge excessive reactive oxygen species (ROS) at the wound site to regulate local microenvironment, including regulation of cytokine express and macrophage polarization, accelerating infected diabetic wound repair, and also avoiding the potential secondary injury.

This study developed a kind of PEG-crosslinked O-carboxymethyl chitosan (O-CMC-PEG) with various PEG content for food packaging. The crosslinking agent of isocyanate-terminated PEG was firstly synthesized by a simple condensation reaction between PEG and excess diisocyanate, then the crosslink between O-carboxymethyl chitosan (O-CMC) and crosslinking agent occurred under mild conditions to produce O-CMC-PEG with a crosslinked structure linked by urea bonds. FT-IR and 1H NMR techniques were utilized to confirm the chemical structures of the crosslinking agent and O-CMC-PEGs. Extensive research was conducted to investigate the impact of the PEG content (or crosslinking degree) on the physicochemical characteristics of the casted O-CMC-PEG films. The results illuminated that crosslinking and components compatibility could improve their tensile features and water vapor barrier performance, while high PEG content played the inverse effects due to the microphase separation between PEG and O-CMC segments. The in vitro degradation rate and water sensitivity primarily depended on the crosslinking degree in comparison with the PEG content. Furthermore, caused by the remaining -NH2 groups of O-CMC, the films demonstrated antibacterial activity against Escherichia coli and Staphylococcus aureus. When the PEG content was 6% (medium crosslinking degree), the prepared O-CMC-PEG-6% film possessed optimal tensile features, high water resistance, appropriate degradation rate, low water vapor transmission rate and fine broad-spectrum antibacterial capacity, manifesting a great potential for application in food packaging to extend the shelf life.

The escalating focus on environmental concerns and the swift advancement of eco-friendly biodegradable batteries raises a pressing demand for enhanced material design in the battery field. The traditional polypropylene (PP) that is monopolistically utilized in the commercial LIBs is hard to recycle. In this work, we prepare a novel water degradable separators via the cross-linking of polyvinyl alcohol (PVA) and dibasic acid (tartaric acid, TA). Through the integration of non-solvent liquid-phase separation, we successfully produced a thermally stable PVA-TA membrane with tunable thickness and a high level of porosity. These specially engineered PVA-TA separators were implemented in LiFePO4 (LFP)|separator|Li cells, resulting in superior multiplicative performance and achieving a capacity of 88 mAh g-1 under 5 C. Additionally, the straightforward small molecule cross-linking technique significantly reduced the crystalline region of the polymer, thereby enhancing ionic conductivity. Notably, after cycling, the PVA-TA separators can be easily dissolved in 95 °C hot water, enabling its reutilization for the production of new PVA-TA separators. Therefore, this work introduces a novel concept to design green and sustainable separators for recyclable lithium batteries.

Image-guided tumor ablative therapies are mainstay cancer treatment options but often require intra-procedural protective tissue displacement to reduce the risk of collateral damage to neighboring organs. Standard of care strategies, such as hydrodissection (fluidic injection), are limited by rapid diffusion of fluid and poor retention time, risking injury to adjacent organs, increasing cancer recurrence rates from incomplete tumor ablations, and limiting patient qualification. Herein, a \"gel-dissection\" technique is developed, leveraging injectable hydrogels for longer-lasting, shapeable, and transient tissue separation to empower clinicans with improved ablation operation windows and greater control. A rheological model is designed to understand and tune gel-dissection parameters. In swine models, gel-dissection achieves 24 times longer-lasting tissue separation dynamics compared to saline, with 40% less injected volume. Gel-dissection achieves anti-dependent dissection between free-floating organs in the peritoneal cavity and clinically significant thermal protection, with the potential to expand minimally invasive therapeutic techniques, especially across locoregional therapies including radiation, cryoablation, endoscopy, and surgery.

Conventional piezoelectric nanogenerators (PNGs) face challenges in terms of degradation and reusability, which have negative environmental implications. On the other hand, biocompatible and degradable piezoelectric materials often exhibit lower piezoelectric response. In this study, potassium sodium niobate (KNN) powder and the biodegradable polymer poly(ε-caprolactone) (PCL) were used to fabricate piezoelectric composite films through solution casting. By constructing staggered electrodes, the total polarized charges quantity is increased, achieving a larger current output. The three-unit PNG (3-PNG) based on the composite film with 15 wt% KNN powder, reaches a maximum output current of 0.85 μA, which exhibits higher charging efficiency compared to 1-PNG. Moreover, the prepared 3-PNG can effectively harvest mechanical energy from human activities and maintain a stable output after 10,000 cycles of bending and releasing. The film exhibits complete degradation when exposed to acidic, neutral, and alkaline solutions. This research provides a promising option for environmentally friendly piezoelectric materials selected and output performance enhanced through optimized structural designs, making them more suitable for practical applications.

Environmentally friendly crosslinked polymer networks feature degradable covalent or non-covalent bonds, with many of them manifesting dynamic characteristics. These attributes enable convenient degradation, facile reprocessibility, and self-healing capabilities. However, the inherent instability of these crosslinking bonds often compromises the mechanical properties of polymer networks, limiting their practical applications. In this context, environmentally friendly dual-crosslinking polymer networks (denoted EF-DCPNs) have emerged as promising alternatives to address this challenge. These materials effectively balance the need for high mechanical properties with the ability to degrade, recycle, and/or self-heal. Despite their promising potential, investigations into EF-DCPNs remain in their nascent stages, and several gaps and limitations persist. This Review provides a comprehensive overview of the synthesis, properties, and applications of recent progress in EF-DCPNs. Firstly, synthetic routes to a rich variety of EF-DCPNs possessing two distinct types of dynamic bonds (i.e., imine, disulfide, ester, hydrogen bond, coordination bond, and other bonds) are introduced. Subsequently, complex structure- and dynamic nature-dependent mechanical, thermal, and electrical properties of EF-DCPNs are discussed, followed by their exemplary applications in electronics and biotechnology. Finally, future research directions in this rapidly evolving field are outlined.

Degradable wearable electronics are attracting increasing attention to weaken or eliminate the negative effect of waste e-wastes and promote the development of medical implants without secondary post-treatment. Although various degradable materials have been explored for wearable electronics, the development of degradable wearable electronics with integrated characteristics of highly sensing performances and low-cost manufacture remains challenging. Herein, we developed a facile, low-cost, and environmentally friendly approach to fabricate a biocompatible and degradable silk fibroin based wearable electronics (SFWE) for on-body monitoring. A combination of rose petal templating and hollow carbon nanospheres endows as-fabricated SFWE with good sensitivity (5.63 kPa-1), a fast response time (147 ms), and stable durability (15,000 cycles). The degradable phenomenon has been observed in the solution of 1 M NaOH, confirming that silk fibroin based wearable electronics possess degradable property. Furthermore, the as-fabricated SFWE have been demonstrated that have abilities to monitor knuckle bending, muscle movement, and facial expression. This work offers an ecologically-benign and cost-effective approach to fabricate high-performance wearable electronics.