Zwitterionic polymer coatings facilitate the formation of hydration layers via electrostatic interactions on their surfaces and have demonstrated efficacy in preventing biofouling. They have emerged as a promising class of marine antifouling materials. However, designing multifunctional, environmentally friendly, and natural products-derived zwitterionic polymer coatings that simultaneously resist biofouling, inhibit protein adhesion, exhibit strong antibacterial properties, and reduce algal adhesion is a significant challenge. This study employed two diisocyanates as crosslinkers and natural urushiol and ethanolamine as raw materials. The coupling reaction of diisocyanates with hydroxyl groups was employed to synthesize urushiol-based precursors. Subsequently, sulfobetaine moieties were introduced into the urushiol-based precursors, developing two environmentally friendly and high-performance zwitterionic-functionalized polyurushiol antifouling coatings, denoted as HUDM-SB and IPUDM-SB. The sulfobetaine-functionalized polyurushiol coating exhibited significantly enhanced hydrophilicity, with the static water contact angle reduced to less than 60°, and demonstrated excellent resistance to protein adhesion. IPUDM-SB exhibited antibacterial efficacy up to 99.9% against common Gram-negative bacteria (E. coli and V. alginolyticus) and Gram-positive bacteria (S. aureus and Bacillus. sp.). HUDM-SB achieved antibacterial efficacy exceeding 95.0% against four bacterial species. Furthermore, the sulfobetaine moieties on the surfaces of the IPUDM-SB and HUDM-SB coatings effectively inhibited the growth and reproduction of algal cells by preventing microalgae adhesion. This zwitterionic-functionalized polyurushiol coating does not contain antifouling agents, making it a green, environmentally friendly, and high-performance biomaterial-based solution for marine antifouling.

Ionic conductive hydrogels have attracted increasing research interest in flexible electronics. However, the limited resilience and poor fatigue resistance of current ionic hydrogels significantly restrict their practical application. Herein, an urushiol-based ionic conductive double network hydrogel (PU/PVA-Li) was developed by one-pot thermal initiation polymerization assisted with freeze–thaw cycling and subsequent LiCl soaking. Such a PU/PVA-Li hydrogel comprises a primary network of covalently crosslinked polyurushiol (PU) and a secondary network formed by physically crosslinked poly(vinyl alcohol) (PVA) through crystalline regions. The obtained PU/PVA-Li hydrogel demonstrates exceptional mechanical properties, including ultrahigh strength (up to 3.4 MPa), remarkable toughness (up to 1868.6 kJ/m³), and outstanding fatigue resistance, which can be attributed to the synergistic effect of the interpenetrating network structure and dynamic physical interactions between PU and PVA chains. Moreover, the incorporation of LiCl into the hydrogels induces polymer chain contraction via ionic coordination, further enhancing their mechanical strength and resilience, which also impart exceptional ionic conductivity (2.62 mS/m) to the hydrogels. Based on these excellent characteristics of PU/PVA-Li hydrogel, a high-performance flexible strain sensor is developed, which exhibits high sensitivity, excellent stability, and reliability. This PU/PVA-Li hydrogel sensor can be effectively utilized as a wearable electronic device for monitoring various human joint movements. This PU/PVA-Li hydrogel sensor could also demonstrate its great potential in information encryption and decryption through Morse code. This work provides a facile strategy for designing versatile, ultrastrong, and tough ionic conductive hydrogels using sustainable natural extracts and biocompatible polymers. The developed hydrogels hold great potential as promising candidate materials for future flexible intelligent electronics.

Marine anti-fouling coatings represent an efficient approach to prevent and control the marine biofouling. However, a significant amount of antifouling agent is added to improve the static antifouling performance of the coatings, which leads to an issue whereby static antifouling performance conflicts with eco-friendly traits. Herein, this work reports an in situ reduction synthesis of silver nanoparticles (AgNPs) within polymers to produce composite coatings, aiming to solve the aforementioned issue. Firstly, urushiol-based benzoxazine monomers were synthesized by the Mannich reaction, using an eco-friendly natural product urushiol and n-octylamine and paraformaldehyde as the reactants. Additionally, AgNPs were obtained through the employment of free radicals formed by phenolic hydroxyl groups in the urushiol-based benzoxazine monomers, achieved by the in situ reduction of silver nitrate in benzoxazine. Then, the urushiol-based benzoxazine/AgNPs composite coatings were prepared by the thermosetting method. AgNPs exhibit broad-spectrum and highly efficient antimicrobial properties, with a low risk to human health and a minimal environmental impact. The composite coating containing a small amount of AgNPs (≤1 wt%) exhibits effective inhibition against various types of bacteria and marine microalgae in static immersion, thereby displaying outstanding antifouling properties. This organic polymer and inorganic nanoparticle composite marine antifouling coating, with its simple preparation method and eco-friendliness, presents an effective solution to the conflict between static antifouling effectiveness and environmental sustainability in marine antifouling coatings.

The economic loss and environmental damage caused by metal corrosion is irreversible. Thus, effective methods, such as coating technologies are used to protect metal surfaces from corrosion. In this work, cardanol-based benzoxazine (CB) was synthesized by a solvent-free method using cardanol, paraformaldehyde and n-octylamine. A cardanol-based benzoxazine copper polymer (CBCP) with good mechanical properties was then prepared by CuCl₂ catalysis and can be cured at room temperature. Subsequently, polyimide corrosion inhibitors with a two-dimensional sheet structure (pyromellitic dianhydride polyimide (PDPI) and 1,4,5,8-naphthalene tetracarboxylic dianhydride polyimide (NDPI)) were designed and prepared. Lastly, PDPI or NDPI was mixed with CBCP to obtain two-dimensional lamellar polyimide/cardanol-based benzoxazine copper polymer composite coatings. The Tafel curves and electrochemical impedance spectroscopy (EIS) measurements showed composite coatings with good corrosion resistance in different corrosive media. Compared to CBCP coating, the anticorrosion performance of the composite coatings improved obviously, especially the coating obtained with 0.5 wt% PDPI. It exhibits a high polarization resistance (3.874 × 10⁹ Ω), a high protection efficiency (99.99% and 97.98%) and low corrosion rate (3.376 × 10⁻⁶ mm year⁻¹). This work suggested a facile and eco-friendly strategy for preparing bio-based anticorrosive composite coatings from low cost and abundant cardanol and polyimide corrosion inhibitors, which will significantly promote their application in metal anticorrosion.

Nanocellulose hydrogels are a crucial category of soft biomaterials with versatile applications in tissue engineering, artificial extracellular matrices, and drug-delivery systems. In the present work, a simple and novel method, involving the self-assembly of cellulose nanocrystals (CNCs) induced by tannic acid (TA), was developed to construct a stable hydrogel (SH-CNC/TA) with oriented porous network structures. The gelation process is driven by the H-bonding interaction between the hydroxyl groups of CNCs and the catechol groups of TA, as substantiated by the atoms in molecules topology analysis and FTIR spectra. Interestingly, the assembled hydrogels exhibited a tunable hierarchical porous structure and mechanical moduli by varying the mass ratio of CNCs to TA. Furthermore, these hydrogels also demonstrate rapid self-healing ability due to the dynamic nature of the H-bond. Additionally, the structural stability of the SH-CNC/TA hydrogel could be further enhanced and adjusted by introducing coordination bonding between metal cations and TA. This H-bonding driven self-assembly method may promote the development of smart cellulose hydrogels with unique microstructures and properties for biomedical and other applications.