Programming Hydrogels with Complex Transient Behaviors via Autocatalytic Cascade Reactions
2022-05-04
发表期刊ACS APPLIED MATERIALS & INTERFACES (IF:8.3[JCR-2023],8.7[5-Year])
ISSN1944-8244
EISSN1944-8252
卷号14期号:17
发表状态已发表
DOI10.1021/acsami.2c03177
摘要It is challenging to design complex synthetic life-like systems that can show both autoevolution and fuel-driven transient behaviors. Here, we report a new class of chemical reaction networks (CRNs) to construct life-like polymer hydrogels. The CRNs are constituted of autocatalytic cascade reactions and fuel-driven reaction networks. The reactions start with only two compounds, that is, thiol of 4-arm-PEG-SH and thiuram disulfides, and undergo thiol oxidation (k(1)), disulfide metathesis (k(2)), and thionate hydrolysis-coupling reactions (k(3)) subsequently, leading to a four-state autonomous transition of sol(I) -> soft gel -> sol(II) -> stiff gel. Moreover, thiuram disulfides can be applied as a fuel to drive the repeated occurrence of metathesis and hydrolysis- coupling reactions, generating dissipative stiff gel sol(II) -> stiff gel cycles. Systematic kinetics studies reveal that the event and lifetime of every transient state could be delicately tailored-up by varying the thiuram disulfide concentration, pH of the system, and thiuram structures. Since the consecutive transient behaviors are precisely predictable, we envision the strategy's potential in guiding the molecular designs of autonomous and adaptive materials for many fields.
关键词programmable materials life-like systems autocatalytic cascade reactions kinetics control system chemistry
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收录类别SCI ; EI ; SCIE
语种英语
资助项目Shanghai Pujiang Program[20PJ1411200] ; National Natural Science Foundation of China[52073175] ; Analytical Instrumentation Center, SPST, ShanghaiTech University[SPST-AIC10112914]
WOS研究方向Science & Technology - Other Topics ; Materials Science
WOS类目Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号WOS:000813030300001
出版者AMER CHEMICAL SOC
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文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/178412
专题物质科学与技术学院_PI研究组_郑宜君组
物质科学与技术学院_PI研究组_杨波组
物质科学与技术学院_硕士生
物质科学与技术学院_博士生
通讯作者Zheng, Yijun
作者单位
1.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
2.Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Key Lab Green Printing, Beijing 100190, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R China
第一作者单位物质科学与技术学院
通讯作者单位物质科学与技术学院
第一作者的第一单位物质科学与技术学院
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Zhang, Jingyi,Liu, Jian,Li, Huizeng,et al. Programming Hydrogels with Complex Transient Behaviors via Autocatalytic Cascade Reactions[J]. ACS APPLIED MATERIALS & INTERFACES,2022,14(17).
APA Zhang, Jingyi.,Liu, Jian.,Li, Huizeng.,Li, Xiaohe.,Zhao, Yuanfeng.,...&Zheng, Yijun.(2022).Programming Hydrogels with Complex Transient Behaviors via Autocatalytic Cascade Reactions.ACS APPLIED MATERIALS & INTERFACES,14(17).
MLA Zhang, Jingyi,et al."Programming Hydrogels with Complex Transient Behaviors via Autocatalytic Cascade Reactions".ACS APPLIED MATERIALS & INTERFACES 14.17(2022).
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