biostudies-literaturePeng XDepartment of Science and Technology of Guangdong ProvinceAoE/M-402/20Health and Medical Research Fund, the Food and Health Bureau, the Government of the Hong Kong Special Administrative RegionGuangdong Science and Technology DepartmentResearch Grants Council of the Hong Kong Special Administration Regione2203890https://www.ebi.ac.uk/biostudies/studies/S-EPMC9631067biostudies-literatureUnknown9(31)Achieving robust underwater adhesion by bioadhesives remains a challenge due to interfacial water. Herein a coacervate-to-hydrogel strategy to enhance interfacial water repulsion and bulk adhesion of bioadhesives is reported. The polyethyleneimine/thioctic acid (PEI/TA) coacervate is deposited onto underwater substrates, which can effectively repel interfacial water and completely spread into substrate surface irregularities due to its liquid and water-immiscible nature. The physical interactions between coacervate and substrate can further enhance interfacial adhesion. Furthermore, driven by the spontaneous hydrophobic aggregation of TA molecules and strong electrostatic interaction between PEI and TA, the coacervate can turn into a hydrogel in situ within minutes without additional stimuAdvanced science (Weinheim, Baden-Wurttemberg, Germany)Coacervate-Derived Hydrogel with Effective Water Repulsion and Robust Underwater Bioadhesion Promotes Wound Healing.PMC963106708190416GRF/14108720GRF/14204618T13-402/17-N2018B030322006GRF/14202920Peng XLi GLi YLi TXie XBian LWang YDeng YfalseCoacervate-Derived Hydrogel with Effective Water Repulsion and Robust Underwater Bioadhesion Promotes Wound Healing.Achieving robust underwater adhesion by bioadhesives remains a challenge due to interfacial water. Herein a coacervate-to-hydrogel strategy to enhance interfacial water repulsion and bulk adhesion of bioadhesives is reported. The polyethyleneimine/thioctic acid (PEI/TA) coacervate is deposited onto underwater substrates, which can effectively repel interfacial water and completely spread into substrate surface irregularities due to its liquid and water-immiscible nature. The physical interactions between coacervate and substrate can further enhance interfacial adhesion. Furthermore, driven by the spontaneous hydrophobic aggregation of TA molecules and strong electrostatic interaction between PEI and TA, the coacervate can turn into a hydrogel in situ within minutes without additional stimu2022-01-01T00:00:00Z2022 Nov2025-04-05T12:33:34.414Z2025-02-19T00:31:37.846ZS-EPMC96310673610918710.1002/advs.202203890