文献类型：期刊文献

英文题名：Harnessing the Hofmeister Effect for Dynamic Self-Assembly of Supramolecular Hydrogels

作者：Tang, Hongwang[1];Gao, Yuliang[1];Zhang, Jiahao[1];Li, Zhongqi[1];Gao, Qi[1];Cai, Peiwen[1];Chen, Xinyu[1];Guo, Xuhong[1];van Esch, Jan H.[3];Wang, Yiming[1,2];Xuan, Fu-Zhen[2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Meilong Rd 130, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Key Lab Intelligent Sensing & Detect Tech, Meilong Rd 130, Shanghai 200237, Peoples R China;[3]Delft Univ Technol, Dept Chem Engn, Van der Maasweg 9, NL-2629 HZ Delft, Netherlands

年份：2025

卷号：64

期号：26

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20251818334216);WOS:【SCI-EXPANDED(收录号:WOS:001477041300001)】；

基金：The authors acknowledge the financial support of the Natural Science Foundation of Shanghai (22ZR1417700), the Science Fund for Creative Research Groups of the Natural Science Foundation of China (52321002 and 21908061), and the Shanghai Pilot Program for Basic Research (22TQ1400100-9). The authors would like to express our gratitude to Prof. Shengtong Sun and Ms. Ying Zhao from Donghua University for their assistance with low-field 1H NMR measurements.

语种：英文

外文关键词：Dynamic gelation; Hofmeister effect; Low-molecular-weight gelators; Self-assembly; Supramolecular chemistry

摘要：Dynamic regulation of intermolecular interactions is essential for the creation of dynamic supramolecular materials with lifelike self-regulating functions. Yet specific ion effect, which is known to possess potent effect on intermolecular interactions, has remained unexplored for such a purpose. Here, we demonstrate our access to dynamic self-assembly of supramolecular hydrogels by orchestrating the Hofmeister effect through a simple enzymatic reaction. The involved gelators containing carboxylate moieties self-assemble into hydrogel (Gel1) at acidic pH and dissolve at basic pH. We surprisingly find that the dissolved gelators at basic pH can be driven to self-assemble into hydrogel (Gel2) by kosmotropic ions through the disruption of gelator-water interactions. By coupling to the enzymatic hydrolysis of urea, Gel1 gradually disintegrates over time because of the production of basic NH3. However, interestingly, with the accumulation of kosmotropic ions, NH4+ and CO32-, the dissolved gelators are driven to self-assemble into Gel2, realizing a self-regulating gel-sol-gel transition process. The transition rate and stiffness of Gel2 are tunable by adjusting the concentrations of urea or urease. This work may shed light on the creation of lifelike self-regulating supramolecular materials using Hofmeister effect for many enticing applications such as ion-programmed biosensing and drug delivery.