Adjacent cationic–aromatic sequences yield strong electrostatic adhesion of hydrogels in seawater
Open accessAbstract
Electrostatic interaction is strong but usually diminishes in high ionic-strength environments. Biosystems can use this interaction through adjacent cationic–aromatic amino acids sequence of proteins even in a saline medium. Application of such specific sequence to the development of cationic polymer materials adhesive to negatively charged surfaces in saline environments is challenging due to the difficulty in controlling the copolymer sequences. Here, we discover that copolymers with adjacent cation–aromatic sequences can be synthesized through cation–π complex-aided free-radical polymerization. Sequence controlled hydrogels from diverse cation/aromatic monomers exhibit fast, strong but reversible adhesion to negatively charged surfaces in seawater. Aromatics on copolymers are found to enhance the electrostatic interactions of their adjacent cationic residues to the counter surfaces, even in a high ionic-strength medium that screens the electrostatic interaction for common polyelectrolytes. This work opens a pathway to develop adhesives using saline water.
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Ideal random copolymerization of the six functional monomers has minimal composition drift during polymerization and enables statistically controlled sequences.
“Therefore, we aimed to statistically replicate the sequence features of functional classes through ideal random copolymerization of the six functional monomers, which has minimal composition drift during polymerization and enables statistically controlled sequences19,27–29.”
From Data-driven de novo design of super-adhesive hydrogels (2025) · cites this paper as [27]
The Results section (page not provided) reports equal incorporation throughout polymerization for certain cationic–aromatic monomer pairs at 1.0 M, supporting minimal composition drift under those conditions. The paper does not establish this for ideal random copolymerization of six functional monomers; its sequence control depends on cation–π interactions and matching vinyl heads. (LLM, conf=0.84)
Experimental — accuracy not yet measuredIdeal random copolymerization of functional monomers (with near-unity reactivity ratios) plays an important role in achieving the statistical sequence features essential for mimicking protein functions.
“This finding underscores the important role of ideal random copolymerization of functional monomers (with near-unity reactivity ratios) in achieving the statistical sequence features essential for mimicking protein functions19,27.”
From Data-driven de novo design of super-adhesive hydrogels (2025) · cites this paper as [27]
The Introduction links adjacent cationic–aromatic sequences to a protein-inspired adhesion mechanism, and the Results report equal incorporation of certain monomer pairs. But the Results attribute that outcome to cation–π interactions and matched vinyl heads, not ideal random copolymerization or near-unity reactivity ratios; the paper does not establish that statistical sequences are essential for mimicking protein functions. Our copy provides section labels but no page numbers. (LLM, conf=0.82)
Experimental — accuracy not yet measuredBA and PEA effectively expel water from the contact interface, and when neighbouring with ATAC, they could enhance electrostatic interactions with the negatively charged glass surface.
“This is because BA and PEA effectively expel water from the contact interface, and, when neighbouring with ATAC (Supplementary Fig. 11), they could enhance electrostatic interactions with the negatively charged glass surface27,40–43 (Supplementary Fig. 12).”
From Data-driven de novo design of super-adhesive hydrogels (2025) · cites this paper as [27]
The Discussion (page unavailable) proposes that an aromatic group adjacent to a cationic group may disrupt the hydration layer, allowing stable electrostatic interaction with glass. The Results report enhanced adsorption of ATAC-adj-PEA on negatively charged SiO₂. The paper supports this mechanism for PEA, but does not establish it for BA, and presents surface dehydration as a proposed mechanism rather than a demonstrated fact. (LLM, conf=0.85)
Experimental — accuracy not yet measuredA crosslinker concentration of 0.1 mol% relative to total monomer content balances the elasticity and deformability of the gels.
“The crosslinker concentration was fixed at 0.1 mol% relative to the total monomer content to balance the elasticity and deformability of the gels27.”
From Data-driven de novo design of super-adhesive hydrogels (2025) · cites this paper as [27]
The Methods (Synthesis of polymer hydrogels; page unavailable) define crosslinker amounts relative to total monomer concentration, and the Results (Figs. 3 and 5; page unavailable) report using 0.1 mol% crosslinker. The paper discusses mechanical strength and deformation, but does not state that 0.1 mol% was chosen to balance elasticity and deformability. (LLM, conf=0.84)
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Self-citation
- Authors
- Fan, H., Wang, J., Tao, Z., Huang, J., Rao, P., Kurokawa, T., & Gong, J. P.
- Affiliations
- Hokkaido University (JP)
- Corresponding author
- Gong, Jian Ping
- Venue
- Nature Communications
- Published
- 2019-11-12
- Volume
- 10
- Issue
- 1
- Pages
- 5127-5127
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC6851134
- OpenAlex
- W2988854674
- Cited by
- 379
- References
- 37
- Citations by year
- 2026: 40 · 2025: 68 · 2024: 77 · 2023: 59 · 2022: 63 · 2021: 53 · 2020: 18
- FWCI
- 10.53
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion)
- Hokkaido University Collection of Scholarly and Academic Papers (Hokkaido University) (submittedVersion, cc-by)
- Institutional Repositories DataBase (IRDB) (submittedVersion, cc-by)
- Funders
- MEXT | Japan Society for the Promotion of Science (JP17H06144)
- Topics
- Physical Sciences › Materials Science › Surfaces, Coatings and Films › Polymer Surface Interaction Studies
- Physical Sciences › Chemistry › Organic Chemistry › Advanced Polymer Synthesis and Characterization
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Electrostatics and Colloid Interactions
- Keywords
- electrostatic adhesion, hydrogels, seawater, cation-π interactions, sequence-controlled polymerization, radical polymerization, polyelectrolytes, high ionic strength, negatively charged surfaces, adhesives
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