具有热/pH 响应性的多酰胺官能化 Y 结聚丙烯酰胺,其热逆性取决于取代基

IF 5.1 1区 化学 Q1 POLYMER SCIENCE Macromolecules Pub Date : 2024-11-27 DOI:10.1021/acs.macromol.4c02080
Meng Zhang, Qingqing Wang, Xin Zhao, Jinqian Zhang, Youliang Zhao
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引用次数: 0

摘要

聚合物的链结构和化学成分在调节热致伸缩特性方面起着至关重要的作用。尽管取得了巨大进步,但要实现具有可调热滞后和超限的 LCST/ 高临界溶液温度(LCST/UCST)特性仍然十分困难。本研究提供了一种很有前景的策略,即通过集成多酰胺和特定取代基来应对这一挑战。在多酰胺功能化 Y 结聚合物(MAYJPs)的每个 Y 结中加入异丙基、2-二乙氨基乙基或氨基甲酰基甲基等两个取代基,可以增强聚合物与聚合物之间的相互作用。氢键、静电相互作用和亲水与疏水比例之间的内在平衡被打破,从而产生了多谐相变。异性取代基的位置转换可导致逆相变或相变温度的显著不同。对亚基水合状态的热力学或动态控制导致出现四种热可逆性,包括轻微或显著的滞后、连续超速和滞后,以及加热-冷却循环时的明显超速。溶剂同位素效应会导致不同类型或不同温度的相变,而 pH 值效应则反映在 pH 值引起的相变温度升高、降低或呈 V 型演变。此外,相变还可能伴随着球体、囊泡、纳米管和薄片之间的形态转变。这些基本发现有助于深入了解与多氨基相关的相变和热可逆性。由于取代基的多样性,MAYJPs 有可能成为具有多用途应用前景的热致伸缩性聚合物。
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Thermo/pH-Responsive Multiamide-Functionalized Y-Junction-Bearing Polyacrylamides with Substituent-Dependent Thermal Reversibility
Chain architecture and chemical composition of polymers can play vital roles in regulating thermoresponsive properties. Despite tremendous progress, it remains difficult to achieve LCST/upper critical solution temperature (LCST/UCST) behavior with tunable thermal hysteresis and outstripping. This study affords a promising strategy of an integrated multiamide and specific substituents to address the challenge. The incorporation of two substituents involving isopropyl, 2-diethylaminoethyl, or carbamoylmethyl into each Y junction of multiamide-functionalized Y-junction-bearing polymers (MAYJPs) allows enhancing polymer–polymer interactions. The disruption of intrinsic balances among hydrogen bonding, electrostatic interactions, and hydrophilic-to-hydrophobic ratio renders a multitunable phase transition. The location switching of heterosubstituents can result in either an inverse phase transition or a significantly different phase transition temperature. The thermodynamic or dynamic control over the hydration status of subunits leads to the occurrence of four kinds of thermal reversibility involving slight or significant hysteresis, consecutive outstripping and hysteresis, and pronounced outstripping upon heating–cooling cycles. The solvent isotope effect results in a distinct type or temperature of phase transition, and the pH effect is reflected in the pH-induced increase, decrease, or V-shaped evolution of phase transition temperature. In addition, the phase transition can accompany morphology transformation among spheres, vesicles, nanotubes, and lamellae. These fundamental findings are beneficial for gaining insights into the multiamide-related phase transition and thermal reversibility. Owing to the diversity of substituents, MAYJPs may serve as promising thermoresponsive polymers for multipurpose applications.
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来源期刊
Macromolecules
Macromolecules 工程技术-高分子科学
CiteScore
9.30
自引率
16.40%
发文量
942
审稿时长
2 months
期刊介绍: Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.
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