Stimuli-Responsive Polymer Film that Autonomously Translates a Molecular Detection Event into a Macroscopic Change in Its Optical Properties via a Continuous, Thiol-Mediated Self-Propagating Reaction
Abstract:This Communication describes a chemically responsive polymer film that is capable of detecting low levels of a specific applied molecular signal (thiol) and subsequently initiating a self-propagating reaction within the material that converts the nonfluorescent film into a globally fluorescent material. We illustrate that the intensity of the resulting fluorescent material is independent of the quantity of the applied thiol, whereas the rate to reach the maximum level of signal is directly proportional to the … Show more
“…超分子材料是当今材料科学研究的热点之一, 其 具有分子间作用特异性结合、操作性强等优点, 因而 也可被用于构筑薄膜基荧光传感器 [66] . 其中, 超分子 20; (c) 自主研制的VSOMs蒸气检测传感平台 [63] (网络版彩图) (3) 与配体 图 10 (a) PFAP的化学结构; (b) PFAP薄膜的发射强度随不同浓度TFA蒸气的变化 [71] (网络版彩图) [30] (网络版彩图) 图 13 当暴露于微量硫醇时, 聚合物薄膜从无荧光完全转 变为荧光形式的机理图 [86] (网络版彩图) Figure 13 Illustration of a polymeric film that transforms completely from nonfluorescent to fluorescent when exposed to trace levels of added thiol [86] (color online). (网络版彩图) 图 15 薄膜制备流程图及PA的检测机理图 [88] (网络版彩图) Figure 15 Schematic diagram of the film casting and the mechanism for the attogram-level detection of PA [88] (color online).…”
“…超分子材料是当今材料科学研究的热点之一, 其 具有分子间作用特异性结合、操作性强等优点, 因而 也可被用于构筑薄膜基荧光传感器 [66] . 其中, 超分子 20; (c) 自主研制的VSOMs蒸气检测传感平台 [63] (网络版彩图) (3) 与配体 图 10 (a) PFAP的化学结构; (b) PFAP薄膜的发射强度随不同浓度TFA蒸气的变化 [71] (网络版彩图) [30] (网络版彩图) 图 13 当暴露于微量硫醇时, 聚合物薄膜从无荧光完全转 变为荧光形式的机理图 [86] (网络版彩图) Figure 13 Illustration of a polymeric film that transforms completely from nonfluorescent to fluorescent when exposed to trace levels of added thiol [86] (color online). (网络版彩图) 图 15 薄膜制备流程图及PA的检测机理图 [88] (网络版彩图) Figure 15 Schematic diagram of the film casting and the mechanism for the attogram-level detection of PA [88] (color online).…”
“…The externally controlled temporary reduction in tensile modulus and/or adhesion strength has been demonstrated for various systems, for example, in supramolecular materials or those containing dynamic covalent bonds. 21 This progress in bottom-up material design has facilitated the immergence of new technologies 22,23 across a broad range of disciplines including biomedical applications, [24][25][26][27] sensors, 28 healable 29 and damage sensing materials 30 as well as improving product recyclability. 25,31,32 With respect to reversible adhesive materials, dynamic covalent chemistries 21 have, to date, received the most attention.…”
A polyurethane-based adhesive has been produced that can undergo multiple thermal debonding/bonding cycles and also irreversibly debond through depolymerisation on contact with fluoride ions.
“…Polymers which can be degraded on command, i.e., upon exposure to a pre-defined external stimulus, are of great interest in the context of recycling, 1 debonding-on-demand adhesives, 2 small molecules release, 3 biomedical applications, 1 sensors, 4 and many other applications. 5,6 To achieve degradability, a variety of concepts have been investigated, including the introduction of chemically labile groups (such as esters or acetals), 7 the design of self-immolative polymers (which undergo depolymerization upon cleavage of stimuli-responsive end-groups), 8 the stimulidriven disassembly of supramolecular polymers, 2 the (dis)assembly of nanoparticles based on polymers exhibiting a lower critical solution temperature (LCST), 9 and the introduction of stimuli-responsive moieties that can be preferentially cleaved upon exposure to a specific stimulus or a combination thereof.…”
ABSTRACT. Molecules comprising aliphatic azo moieties are widely used as radical polymerization initiators, but only few studies have explored their usefulness as stimuliresponsive motifs in macromolecular constructs. The controlled degradation of azo-containing polymers has indeed remained largely unexplored. Here we present the syntheses of linear azocontaining polyamides and polyurethanes and report on their thermally and optically induced responses in solution and the solid state. We show that the stimuli-induced degradation behavior depends strongly on the nature of the polymer backbone, the state of matter, and in solution, on the nature of the solvent. The stimuli-responsive solid-state properties of the azo-containing materials may be particularly useful. In the case of the polyurethanes studied here, temperatureor light-induced cleavage of the azo motifs led to a controllable decrease of the molecular weight, which in turn caused a reduction of the elongation at break, modulus and strength. The controlled degradation of the polymer in well-defined areas can be readily achieved via photopatterning, and this approach was shown to be useful to produce solid structures with graded mechanical properties.2
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