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The adhesion of marine organisms to marine facilities negatively impacts human productivity. This phenomenon, known as marine fouling, constitutes a serious issue in the marine equipment industry. It increases resistance for ships and their structures, which, in turn, raises fuel consumption and reduces ship speed. To date, numerous antifouling strategies have been researched to combat marine biofouling. However, a multitude of these resources face long-term usability issues due to various limitations, such as low adhesion quality, elevated costs, and inefficacy. Hydrogels, exhibiting properties akin to the slime layer on the skin of many aquatic creatures, possess a low frictional coefficient and a high rate of water absorbency and are extensively utilized in the marine antifouling field. This review discusses the recent progress regarding the application of hydrogels as an important marine antifouling material in recent years. It introduces the structure, properties, and classification of hydrogels; summarizes the current research status of improved hydrogels in detail; and analyzes the improvement in their antifouling properties and the prospects for their application in marine antifouling.

With the increasing awareness of environmental protection, it is necessary to develop natural product extracts as antifouling (AF) agents for alternatives to toxic biocides or metal-based AF paints to control biofouling. This paper briefly summarizes the latest developments in the natural product extracts and their derivatives or analogues from marine microorganisms to terrestrial plants as AF agents in the last five years. Moreover, this paper discusses the structures–activity relationship of these AF compounds and expands their AF mechanisms. Inspired by the molecular structure of natural products, some derivatives or analogues of natural product extracts and some novel strategies for improving the AF activity of protective coatings have been proposed as guidance for the development of a new generation of environmentally friendly AF agents.

Benzoxazine resins are new thermosetting resins with excellent thermal stability, mechanical properties, and a flexible molecular design, demonstrating promise for applications in marine antifouling coatings. However, designing a multifunctional green benzoxazine resin-derived antifouling coating that combines resistance to biological protein adhesion, a high antibacterial rate, and low algal adhesion is still challenging. In this study, a high-performance coating with a low environmental impact was synthesized using urushiol-based benzoxazine containing tertiary amines as the precursor, and a sulfobetaine moiety into the benzoxazine group was introduced. This sulfobetaine-functionalized urushiol-based polybenzoxazine coating (poly(U−ea/sb)) was capable of clearly killing marine biofouling bacteria adhered to the coating surface and significantly resisting protein attachment. poly(U−ea/sb) exhibited an antibacterial rate of 99.99% against common Gram negative bacteria (e.g., Escherichia coli and Vibrio alginolyticus) and Gram positive bacteria (e.g., Staphylococcus aureus and Bacillus sp.), with >99% its algal inhibition activity, and it effectively prevented microbial adherence. Here, a dual-function crosslinkable zwitterionic polymer, which used an “offensive-defensive” tactic to improve the antifouling characteristics of the coating was presented. This simple, economic, and feasible strategy provides new ideas for the development of green marine antifouling coating materials with excellent performance.

Superhydrophobic surfaces have demonstrated exceptional efficacy in combatting biofouling contaminations of optical devices and equipment in marine applications. However, the fabrication of highly transparent superhydrophobic materials remains a formidable challenge due to the inherent trade-off between surface roughness for superhydrophobicity and optical transparency. Herein, we design a robust and transparent superhydrophobic coating (Si-POSS) embedded silica nanoparticles (200 nm) with fluorinated polyhedral oligomeric silsesquioxanes (F-POSS) and zinc pyrithione (ZPT). The Si-POSS coating exhibits excellent water repellence toward diverse liquids and optical transmittance exceeding 90% in the visible spectrum. Moreover, the Si-POSS coating sustains long-term anti-bacterial (> 99.11%) and anti-algal effects for over 30 days, accompanied by mechanical, chemical, and thermal stability. This research asserts that the Si-POSS coating with outstanding combined characteristics holds significant potential for marine applications, particularly in self-cleaning and antifouling endeavors.

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.

Marine fouling on concrete has become one of the severest problems that damage the surface and even cause internal corrosion of marine concrete. Dissimilarly to the previous abuse of toxic antifoulants, developing hydrophobic waterborne antifouling materials could be regarded as one of the most environment-friendly and potential directions to protect marine concrete. However, the insufficient hydrophobicity, antifouling, and mechanical properties limit their application. Herein, we reported a series of hybrid coatings combining hyperbranched polyglycerol (HPG) decorated waterborne fluoro silicone polyurethane (H) and HPG-grafted graphene oxide (G-HPG) that improve the hydrophobicity, antifouling, and mechanical properties. The hybrid materials were modified by the hyperbranched polyglycerol synthesized based on the anionic-ring-opening reaction between glycerol and ethylene glycol or polyethylene glycol. Remarkably, the hydrophobicity (115.19°) and antifouling properties (BSA absorption of 2.33 μg/cm2 and P. tricornutum attachment of 1.289 × 104 CFU/cm2) of the materials could be developed by the modification of HPG with higher generation numbers and backbone molecular weights. Moreover, the mechanical properties negligibly decreased (tensile strength decreased from 11.29 MPa to 10.49 MPa, same pencil hardness and adhesion grade as H of 2H and grade 2). The results revealed that the HPG of higher generation numbers and backbone molecular weights could benefit materials with enhanced antifouling properties and hydrophobicity. The method of hyperbranched modification can be regarded as potentially effective in developing the durability and antifouling properties of marine antifouling materials.

Marine biofouling is an urgent global problem in the process of ocean exploitation and utilization. In our work, a series of zinc-based acrylate copolymers (ACZn-x) were designed and synthesized using benzoic acid, zinc oxide (ZnO) and a random quaternion copolymer consisting of ethyl acrylate (EA), butyl acrylate (BA), acrylic acid (AA) and methacrylic acid (MAA) by free radical polymerization and dehydration condensation. The ACZn-x with a zinc benzoate side chain is able to hydrolyze in natural seawater under static conditions, resulting in the formation of a smooth surface. We investigated and confirmed the antifouling (AF) behavior of ACZn-x in the laboratory and revealed that they have better antibacterial (86% for S. aureus and 72% for E. coli ) and anti-algal (≥60.1% for N. closterium and ≥67.5% for P. subcordiformis ) activities. We also assessed the marine AF properties of ACZn-x and corresponding coatings in Qingdao, China; the ACZn-x exhibited ideal AF properties with little silt and biological mucosa adhered to the ACZn-x surface after 6 months, and corresponding coatings exhibited little biofouling after 16 months in the ocean. Importantly, possible AF mechanisms were further proposed at the cellular level. These results could be helpful for the development and application of effective AF coatings.

Marine biofouling–the adhesion of marine organisms onto a ship hull–causes increased fuel consumption, leading to massive carbon dioxide emissions. Many attempts are made to address this issue, and antifouling polymer coatings are extensively investigated owing to their environmental friendliness. Zwitterionic polymers, polysaccharides, and polyethylene glycol are frequently used as surface coatings, demonstrating excellent marine antifouling performance. However, these hydrophilic polymer coatings have a major drawback: when exposed to sediment, various minerals are easily adsorbed by the coatings, causing them to lose their inherent antifouling properties. Amphiphilic polymer coatings have therefore been proposed as alternatives to hydrophilic polymer coatings. In this study, the synthesis of amphiphilic copolymers composed of carboxybetaine methacrylamide and trifluoroethyl methacrylate and the immobilization of these copolymers onto solid surfaces are reported. This method utilizes material‐independent surface‐coating properties and the metal complex‐forming ability of polydopamine to immobilize amphiphilic copolymers onto solid surfaces. The resulting surfaces exhibit good antifouling performance against both diatom adhesion and silt adsorption. As this is a facile and substrate‐independent method for immobilizing polymers, an expectation exists for it to be an effective platform for the coating of new marine antifouling polymers. The synthesis of amphiphilic copolymers composed of carboxybetaine methacrylamide and trifluoroethyl methacrylate and the immobilization of these copolymers onto glass and stainless‐steel surfaces are reported. This method utilizes material‐independent surface‐coating properties and the metal complex‐forming ability of polydopamine to immobilize amphiphilic copolymers onto solid substrates. The amphiphilic copolymer coatings exhibit good antifouling performance against both diatom adhesion and silt adsorption.

Marine biofouling is a worldwide problem in coastal areas and affects the maritime industry primarily by attachment of fouling organisms to solid immersed surfaces. Biofilm formation by microbes is the main cause of biofouling. Currently, application of antibacterial materials is an important strategy for preventing bacterial colonization and biofilm formation. A natural three-dimensional carbon skeleton material, TRP (treated rape pollen), attracted our attention owing to its visible-light-driven photocatalytic disinfection property. Based on this, we hypothesized that TRP, which is eco-friendly, would show antifouling performance and could be used for marine antifouling. We then assessed its physiochemical characteristics, oxidant potential, and antifouling ability. The results showed that TRP had excellent photosensitivity and oxidant ability, as well as strong anti-bacterial colonization capability under light-driven conditions. Confocal laser scanning microscopy showed that TRP could disperse pre-established biofilms on stainless steel surfaces in natural seawater. The biodiversity and taxonomic composition of biofilms were significantly altered by TRP (p < 0.05). Moreover, metagenomics analysis showed that functional classes involved in the antioxidant system, environmental stress, glucose–lipid metabolism, and membrane-associated functions were changed after TRP exposure. Co-occurrence model analysis further revealed that TRP markedly increased the complexity of the biofilm microbial network under light irradiation. Taken together, these results demonstrate that TRP with light irradiation can inhibit bacterial colonization and prevent initial biofilm formation. Thus, TRP is a potential nature-based green material for marine antifouling.

Polyurethane coating materials with different compositions of low surface energy polydimethylsiloxane and degradable poly( l -lactic acid) were synthesized by three major steps. Initially, the hydroxylation-terminated poly( l -lactide)-functionalized graphene (G- g -PLLA) was prepared by ring-opening polymerization of l -lactic acid using the phenol-functionalized graphene (G-f-OH), which was prepared by 1,3-dipolar cycloaddition reaction of graphene and 3,4-dihydroxybenzaldehyde when N -methylglycine and tin octoate were used as initiator and catalyst, respectively. Subsequently, isocyanate-terminated polyurethane prepolymer with polydimethylsiloxane was obtained by condensation polymerization of polydimethylsiloxane and isocyanate-terminated polyurethane prepolymer that was obtained by the condensation polymerization of 4,4′-diphenylmethane diisocyanate and 1,4-butane diol. Finally, the novel polyurethane coating materials were prepared by the condensation polymerization of G- g -PLLA and isocyanate-terminated polyurethane prepolymer with polydimethylsiloxane. These synthesized materials were carefully analyzed with Fourier transform infrared spectroscopy (FTIR), proton nuclear magnetic resonance spectra ( 1 H NMR), field-emission scanning electron microscopy (SEM), and high-resolution transmission (TEM). In addition, the water contact angles were measured. It was found that the surface free energy of the polyurethane coating materials decreased from 52.19 to 11.74 N/m 2 with the increase of polydimethylsiloxane content from 0 to 20% and the water contact angle of the polyurethane coating materials increased from 71° to 108°. Moreover, the mechanical property was investigated. The studies also demonstrated that functionalized polyurethane was able to hydrolyze in seawater and the hydrolysis rate decreased as the PDMS content increased. At the same time, simulative ocean hanging plate experiment confirmed that the novel polyurethane coating materials exhibited a good antifouling performance, which indicated that the functionalized polyurethane has a potentiality in marine antifouling coating application.