Yu Yan, Xiaonong Zhang*, Chunsheng Xiao* and Xuesi Chen*,
{"title":"具有ph可调动态特性的Knoevenagel缩合反应增强水凝胶","authors":"Yu Yan, Xiaonong Zhang*, Chunsheng Xiao* and Xuesi Chen*, ","doi":"10.1021/acsmacrolett.5c0021810.1021/acsmacrolett.5c00218","DOIUrl":null,"url":null,"abstract":"<p >Dynamic hydrogels have found extensive applications in various biomedical fields owing to their remarkable dynamic properties, such as fast stress relaxation and self-healing capabilities. In this work, we report the development of a hydrogel empowered by the reversible Knoevenagel condensation (KC) reaction featuring pH-tunable dynamic properties. By adjusting the pH, the exchange rates and quantities of the dynamic C═C bonds formed via the KC reaction can be regulated through modulation of the association rate constant (<i>k</i><sub>1</sub>), dissociation rate constant (<i>k</i><sub>–1</sub>), and equilibrium constant (<i>K</i><sub>eq</sub>) of the reversible KC reaction. Specifically, pH reduction decelerated both <i>k</i><sub>1</sub> and <i>k</i><sub>–1</sub> of the KC reaction while elevating the <i>K</i><sub>eq</sub>. As a result, when the pH decreased from 10 to 1, the KC reaction-formed dynamic hydrogels exhibited a progressive increase in relaxation time (τ<sub>1/2</sub>) from 100 to over 1,000 s, accompanied by enhanced structural stability and improved mechanical performance. This study provides a new strategy to design the dynamic hydrogels with tunable dynamic properties through the pH-responsive KC reaction.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 6","pages":"773–780 773–780"},"PeriodicalIF":5.2000,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Knoevenagel Condensation Reaction-Empowered Hydrogels with pH-Tunable Dynamic Properties\",\"authors\":\"Yu Yan, Xiaonong Zhang*, Chunsheng Xiao* and Xuesi Chen*, \",\"doi\":\"10.1021/acsmacrolett.5c0021810.1021/acsmacrolett.5c00218\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Dynamic hydrogels have found extensive applications in various biomedical fields owing to their remarkable dynamic properties, such as fast stress relaxation and self-healing capabilities. In this work, we report the development of a hydrogel empowered by the reversible Knoevenagel condensation (KC) reaction featuring pH-tunable dynamic properties. By adjusting the pH, the exchange rates and quantities of the dynamic C═C bonds formed via the KC reaction can be regulated through modulation of the association rate constant (<i>k</i><sub>1</sub>), dissociation rate constant (<i>k</i><sub>–1</sub>), and equilibrium constant (<i>K</i><sub>eq</sub>) of the reversible KC reaction. Specifically, pH reduction decelerated both <i>k</i><sub>1</sub> and <i>k</i><sub>–1</sub> of the KC reaction while elevating the <i>K</i><sub>eq</sub>. As a result, when the pH decreased from 10 to 1, the KC reaction-formed dynamic hydrogels exhibited a progressive increase in relaxation time (τ<sub>1/2</sub>) from 100 to over 1,000 s, accompanied by enhanced structural stability and improved mechanical performance. This study provides a new strategy to design the dynamic hydrogels with tunable dynamic properties through the pH-responsive KC reaction.</p>\",\"PeriodicalId\":18,\"journal\":{\"name\":\"ACS Macro Letters\",\"volume\":\"14 6\",\"pages\":\"773–780 773–780\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2025-05-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Macro Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsmacrolett.5c00218\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"POLYMER SCIENCE\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Macro Letters","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsmacrolett.5c00218","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
Knoevenagel Condensation Reaction-Empowered Hydrogels with pH-Tunable Dynamic Properties
Dynamic hydrogels have found extensive applications in various biomedical fields owing to their remarkable dynamic properties, such as fast stress relaxation and self-healing capabilities. In this work, we report the development of a hydrogel empowered by the reversible Knoevenagel condensation (KC) reaction featuring pH-tunable dynamic properties. By adjusting the pH, the exchange rates and quantities of the dynamic C═C bonds formed via the KC reaction can be regulated through modulation of the association rate constant (k1), dissociation rate constant (k–1), and equilibrium constant (Keq) of the reversible KC reaction. Specifically, pH reduction decelerated both k1 and k–1 of the KC reaction while elevating the Keq. As a result, when the pH decreased from 10 to 1, the KC reaction-formed dynamic hydrogels exhibited a progressive increase in relaxation time (τ1/2) from 100 to over 1,000 s, accompanied by enhanced structural stability and improved mechanical performance. This study provides a new strategy to design the dynamic hydrogels with tunable dynamic properties through the pH-responsive KC reaction.
期刊介绍：
ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science.
With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.
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