Dong Zhi, Wu Jiang, Shen Xinyi, Hua Zan, Liu Guangming
Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China Hefei Anhui 230026 China
Biomass Molecular Engineering Center and Department of Materials Science and Engineering, Anhui Agricultural University Hefei Anhui 230036 China
Chem Sci. 2023 Mar 17;14(14):3938-3948. doi: 10.1039/d3sc00697b. eCollection 2023 Apr 5.
Supramolecular polymeric adhesives inspired by nature have been strongly pursued by scientists, since they possess strong but dynamic reversible adhesive behaviors concurrently. Optimizing the adhesive and cohesive properties is of vital importance for the fabrication of strong supramolecular polymeric adhesives, but common strategies often strengthen one property at the expense of another. Herein, counterion exchange of nucleobase-containing polyelectrolyte adhesives was utilized to boost the interfacial adhesion without compromising the intermolecular cohesion, achieving high adhesion strengths. By employing the cationic polyelectrolyte poly(3-acrylamidopropyltrimethylammonium chloride), the slightly enhanced intermolecular cohesion of the polyelectrolyte with hydrophobic sulfonates is capable of enhancing the adhesion strength. Intriguingly, by introducing bioinspired complementary nucleobases within adhesives, the loss of interfacial adhesion was observed for adhesives containing high supramolecular hydrogen-bonding crosslinking densities. By optimizing the cohesive and adhesive properties of nucleobase-containing polyelectrolyte adhesives using sulfonates with suitable chain lengths, 60 to 250 times improvement of adhesion strengths can be attained over that of initial supramolecular polymeric adhesives. Additionally, nucleobase-containing supramolecular polymeric adhesives tolerate different external conditions, maintaining robust adhesion strengths. This work offers us an efficient and feasible way to optimize the cohesive and adhesive properties for constructing robust and tunable supramolecular adhesives.
受自然启发的超分子聚合物粘合剂一直受到科学家们的强烈追捧，因为它们同时具有强大但动态可逆的粘附行为。优化粘合剂的粘附性和内聚性对于制备强力超分子聚合物粘合剂至关重要，但常见策略往往会以牺牲另一种性能为代价来增强一种性能。在此，利用含核碱基的聚电解质粘合剂的抗衡离子交换来提高界面粘附力，同时不损害分子间内聚力，从而实现高粘附强度。通过使用阳离子聚电解质聚（3-丙烯酰胺基丙基三甲基氯化铵），聚电解质与疏水性磺酸盐之间略微增强的分子间内聚力能够提高粘附强度。有趣的是，通过在粘合剂中引入受生物启发的互补核碱基，观察到含有高超分子氢键交联密度的粘合剂的界面粘附力有所损失。通过使用具有合适链长的磺酸盐优化含核碱基的聚电解质粘合剂的内聚性和粘附性，与初始超分子聚合物粘合剂相比，粘附强度可提高60至250倍。此外，含核碱基的超分子聚合物粘合剂能够耐受不同的外部条件，保持强大的粘附强度。这项工作为我们提供了一种有效且可行的方法，用于优化内聚性和粘附性，以构建坚固且可调的超分子粘合剂。
