Most adhesives lose adhesion in the presence of water. Here, hydrophobic perfluoropolyether (PFPE) dynamic polymers with periodically embedded hydrogen bonding units operate as effective underwater adhesives by enhancing van der Waals interactions and minimizing bulk water uptake. Optimizing the bonding interactions in the polymers and their bulk dynamics enables high cohesive strength while maintaining a hydrophobic, nanophase-separated morphology to prevent water-based failure mechanisms. The resulting adhesives have high adhesion strength and can be reversibly applied in fully underwater conditions to polyimide, glass, and steel substrates without any solvent or covalent crosslinking, at room temperature, and without substrate modifications. Moreover, the polymer adhesive can be readily recycled due to the use of dynamic crosslinking to achieve adhesion. This work shows how dynamic PFPE polymers with tunable structures and properties can be designed for high-strength recyclable underwater adhesives, which could enable reversibly attachable and detachable waterproof wearable devices.

大多数粘合剂在有水的情况下会失去粘合力。在这里，具有周期性嵌入氢键单元的疏水性全氟聚醚（PFPE）动态聚合物通过增强范德华相互作用并最大限度地减少大量水的吸收，可作为有效的水下粘合剂。优化聚合物中的键合相互作用及其整体动力学，可实现高内聚强度，同时保持疏水性、纳米相分离的形态，以防止水基失效机制。所得粘合剂具有高粘合强度，并且可以在完全水下条件下可逆地涂覆到聚酰亚胺上、玻璃和钢基材，无需任何溶剂或共价交联，在室温下，且无需基材改性。此外，由于使用动态交联来实现粘合，聚合物粘合剂可以容易地回收利用。这项工作展示了如何设计具有可调结构和性能的动态 PFPE 聚合物用于高强度可回收水下粘合剂，从而实现可逆连接和可拆卸的防水可穿戴设备。