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Tuning Electrochemiluminescence in Multistimuli Responsive Hydrogel Films
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-01-08 00:00:00 , DOI: 10.1021/acs.jpclett.7b03119
Haidong Li 1 , Silvia Voci 1 , Valérie Ravaine 1 , Neso Sojic 1
Affiliation  

Luminescent and redox properties of stimuli-responsive hydrogel materials have been modulated by different external stimuli which trigger swelling or collapse of the polymer matrix. There is very rapid development in the field of such “smart” materials particularly combined with other sensing functionalities. Here, a poly(N-isopropylacrylamide) matrix incorporating covalently bound phenylboronic acids as a saccharide-sensing unit and redox-active [Ru(bpy)3]2+ luminophores was designed and exhibited multistimuli responsive electrochemical and luminescent switching behaviors. Redox activity of the films is reversibly changed by sequential stimuli (fructose and temperature) which control the swelling and the collapse of the films. Finally, electrogenerated chemiluminescence (ECL) is enhanced by a ∼16-fold factor during the film collapse induced by the temperature, whereas the swelling due to fructose provokes the decrease of the light emission. We demonstrate for the first time that ECL response correlates intrinsically with the swelling ratio and is finely modulated by both stimuli. The multistimuli responsive characteristics of such ECL-active hydrogels should find promising applications in biosensing, new luminescent materials, and logic gates in bioelectronic devices.

中文翻译:

调节多刺激响应水凝胶膜中的化学发光

刺激响应性水凝胶材料的发光和氧化还原特性已通过触发聚合物基质膨胀或塌陷的不同外部刺激来调节。在这种“智能”材料领域,特别是与其他传感功能相结合的领域,发展非常迅速。在这里,聚(N-异丙基丙烯酰胺)基质结合了共价键合的苯基硼酸作为糖敏感单元和氧化还原活性[Ru(bpy)3 ] 2+设计了发光体并表现出多刺激响应的电化​​学和发光转换行为。薄膜的氧化还原活性可通过顺序刺激(果糖和温度)来可逆地改变,所述顺序刺激控制薄膜的溶胀和塌陷。最后,在温度引起的薄膜塌陷过程中,电致化学发光(ECL)增强了约16倍,而果糖引起的溶胀则导致了发光量的减少。我们首次证明,ECL反应与肿胀率内在相关,并且受到两种刺激的调节。这种ECL活性水凝胶的多刺激响应特性应该在生物传感,新型发光材料和生物电子设备中的逻辑门中找到有前途的应用。
更新日期:2018-01-08
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