adhesive, causing plasticization, swelling, erosion, degradation, or hydrolysis of adhesives, which eventually leads to cohesive failure. [8,9] Therefore, the development of underwater adhesives remains a significant challenge.An efficient way of developing underwater adhesives is by taking inspiration from nature. For instance, sessile marine organisms such as mussels and sandcastle worms use L-3,4-dihydroxyphenylalanine (DOPA) to achieve permanent underwater adhesion, whereas aquatic creatures such as remora and clingfish use unique microstructures for temporary underwater attachment. [10][11][12][13] Inspired by these unique underwater adhesion strategies, significant progress has been made in the design and fabrication of novel underwater adhesives in the past decade.Previous reviews on underwater adhesion have mainly focused on the micromechanics and bonding mechanisms. Adhesives for soft and wet tissues and hydrogels have been discussed in other recent reviews. [1,[14][15][16] However, only a few have been devoted to bulk underwater adhesives. [10,12,13,[16][17][18][19][20] In this review, we summarize the currently reported adhesives that show macroscopic adhesion to mainly, but not limited to, solid surfaces under wet and underwater conditions. We provide an overview of the development and performance of underwater adhesives based on different bonding methods and mechanisms. In addition, we discuss the possible research directions and perspectives for underwater adhesives.
Current Design Strategies for Underwater AdhesionThe keys to achieving wet adhesion are the breaking down of the hydration layer and interaction with the substrate surface, which can be designed at different length scales (Figure 1). [21][22][23] To achieve dehydration at the molecular level (∼nm), hydrophobic organic solvents, monomers, and polymers have been used to remove the hydration layer and facilitate surface wetting, especially for hydrophobic substrates. [24,25] The use of water-absorbing fillers, including inorganic substances and hydrophilic polymers, is an alternative strategy that is widely used for wet surfaces. [26][27][28] At a larger length scale (μm to mm), surface microstructures can promote water drainage to prevent permanent water trapping. [29] Accompanied by the dehydration process, the interfacial bonding of adhesives is achieved by the formation of covalent/ non-covalent bonds (∼nm), which highly depends on the interfacial chemistry between the adherend and the adhesive. [10] For Underwater adhesives are in high demand in both commercial and industrial sectors. Compared with adhesives used in dry (air) environments, adhesives used for wet or submerged surfaces in aqueous environments have specific challenges in development and performance. In this review, focus is on adhesives demonstrating macroscopic adhesion to wet/underwater substrates. The current strategies are first introduced for different types of underwater adhesives, and then an overview is provided of the development and performance of underwater ad...