Non‐sticking droplets wrapped with fine hydrophobic particles, namely liquid marbles, can be transported both on solid and water pool without an undesired spill of the inner encapsulated liquid. While the stimuli‐responsive release of the inner liquid in the target area is proposed, the time‐programmed release is not yet achieved. Herein, the hydrophobicity of nanoclay is modulated via a catalyst‐free 1,4‐conjugate addition reaction to form liquid marbles. This nanoclay liquid marble is robust and stable in air but collapses on the liquid pool with a specific lifetime. The lifetime of the liquid marble can be modulated over seconds to hours scale depending on the selection of chemically modulated wettability of the nanoclay. The critical mechanism of lifetime modulation is responsible for controlling the coalescence kinetics between the water pool and inner liquid by nanoclays’ high diffusion length and chemically varied water spreading potential. The NC liquid marble's programmable lifetime to ‘time‐bomb’ type drug release and cascade chemical reaction is applied—without requiring any external intervention.
The inherent ability of bio‐inspired underwater superoleophobicity to prevent oil/oily fouling underwater makes it appropriate for a wide range of applications related to environmental remediation, bio‐adhesion, microfluidics, chemical sensing, etc.; however, the co‐association of mechanical durability and optical transparency is essential for realistic performance. While the design of mechanically durable and absolutely optically transparent underwater superoleophobic coating remains challenging, here, a covalently cross‐linked and chemically reactive sol‐gel conversion process is introduced through 1,4‐conjugate addition reaction to achieve a substrate‐independent and tolerant coating for orthogonally modulating the underwater oil wettability, optical transparency, and even mechanical properties of highly deformable porous and fibrous substrates. The post‐modification of residual chemical reactivity in the prepared coating allows to embed underwater superoleophobicity, and the β‐amino‐ester‐cross‐links improve the mechanical property of selected deformable substrates. Moreover, it displayed unperturbed performance even after prolonged (30 days) exposures in practically relevant chemically harsh aquatic conditions—including extremes of pH, artificial seawater, surfactant contaminated water, etc. The approach is successfully applied to coat various substrates—including porous, fibrous, and planar objects, and it would be useful in protecting various relevant marine infrastructures from oil/oily fouling, and various other potential applications.
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