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From the functionalization of polyelectrolytes to the development of a versatile approach to the synthesis of polyelectrolyte multilayer films with enhanced stability
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2017-11-03 00:00:00 , DOI: 10.1039/c7ta06855g
Thi-Thanh-Tam Nguyen 1, 2, 3, 4, 5 , Sabrina Belbekhouche 1, 2, 3, 4, 5 , Pierre Dubot 1, 2, 3, 4, 5 , Benjamin Carbonnier 1, 2, 3, 4, 5 , Daniel Grande 1, 2, 3, 4, 5
Affiliation  

A general approach to side-chain allyl-functionalization of three different polyelectrolytes (PEs), namely poly(allylamine hydrochloride) (PAH·HCl), branched polyethyleneimine (PEI) and poly(sodium 4-styrenesulfonate) (PSS), is reported for the first time. This functionalization does not affect the electrolytic properties of the newly functionalized PEs (named PEs-ene), as confirmed by the effective formation of PE-ene multilayer (PEM) films. The stepwise construction of these films is monitored using different techniques, including QCM, SEM, XPS, and WCA measurements. The incorporation of allyl functional groups into the PE side-chains allows for the stabilization of the resulting PEM films via thiol–ene UV photo-crosslinking in the presence of a water-soluble dithiol crosslinker. To overcome the problem of film delamination, the covalent crosslinking occurs not only between different layers of PEM films but also with the substrates preliminarily functionalized with allyl functional groups either via sulfur–gold chemistry or via chemical reduction of aryldiazonium salts using two newly synthesized anilinium derivatives. The stability of the resulting crosslinked PEM films in a strongly alkaline solution (pH = 14) is validated on gold substrates under QCM conditions (from 30 min to 3 h), while XPS and WCA measurements are used for evidencing such a stability under strongly acidic conditions (pH = 1) or at high salt concentration (saturated NaCl solution) on a modified anion-exchange membrane during a longer study time, i.e. 10 days. Finally, this stability study also gives evidence for a greater crosslinking efficiency of PEG-diSH, namely a macromolecular crosslinker, over dithiothreitol (DTT), a small molecule. The versatility and effectiveness of the approach presented here are expected to find widespread interest in different fields of emerging applications.

中文翻译:

从聚电解质的功能化到通用方法的发展,以合成具有增强稳定性的聚电解质多层膜

据报导,三种不同的聚电解质(PEs),即聚(烯丙胺盐酸盐)(PAH·HCl),支链聚乙烯亚胺(PEI)和聚(4-苯乙烯磺酸钠)(PSS)的侧链烯丙基官能化的通用方法。第一次。如有效形成PE-烯多层(PEM)膜所证实的,这种官能化不影响新官能化的PEs(称为PEs-ene)的电解性能。使用不同的技术(包括QCM,SEM,XPS和WCA测量)监控这些薄膜的逐步构造。烯丙基官能基团引入到PE侧链的引入允许所得PEM膜的稳定化通过水溶性二硫醇交联剂存在下的硫醇-烯紫外光交联。为了克服薄膜分层的问题,共价交联不仅发生在PEM薄膜的不同层之间,而且还通过硫-金化学反应或通过使用两种新合成的苯胺衍生物化学还原芳基重氮盐。所得交联PEM膜在强碱性溶液(pH = 14)中的稳定性在QCM条件下(30分钟至3小时)在金基底上得到验证,而XPS和WCA测量用于证明在强酸性条件下的这种稳定性。条件(pH = 1)或在较长的研究时间内,在改性的阴离子交换膜上处于高盐浓度(饱和NaCl溶液)的情况下,10天。最后,该稳定性研究还提供了PEG-diSH(即大分子交联剂)比小分子二硫苏糖醇(DTT)更高的交联效率的证据。预期本文介绍的方法的多功能性和有效性会在新兴应用程序的不同领域中引起广泛的关注。
更新日期:2017-11-16
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