Dynamics and Self-Healing of Layer-by-Layer Hydrogen-Bonded Films of Linear Synthetic Polyphenols
Dynamics and Self-Healing of Layer-by-Layer Hydrogen-Bonded Films of Linear Synthetic Polyphenols
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线性合成多酚层层氢键薄膜的动力学和自修复
DOI：
10.1021/acs.macromol.1c01090
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发表时间：
2021
期刊：
影响因子：
5.5
通讯作者：
Sukhishvili, Svetlana
中科院分区：
文献类型：
--
作者：
Hlushko, Raman;Ankner, John F.;Sukhishvili, Svetlana
这项工作探索了具有不同主链和侧基结构的线性合成多酚（lPPh）的氢键层层（LbL）薄膜的动力学。该聚合物具有类儿茶酚或类没食子酚环的重复单元，即聚（3,4-二羟基苄基甲基丙烯酰胺）（P2HMA）、聚（3,4-二羟基苄基丙烯酰胺）（P2HAA）、聚（3,4,5-三羟基苄基丙烯酰胺）（P3HAA）和聚（3,4,5-三羟基苄基甲基丙烯酰胺） （P3HMA），并与线性聚（环氧乙烷）（PEO）组装。 lPPh 的结构对 LbL 薄膜的扩散率有重大影响，并且在薄膜构建过程中，lPPh 和 PEO 封端的薄膜的链动力学是不对称的。具体而言，通过原位脂质光度法评估，对于 P2 和 P3 家族的 lPPh，多酚在垂直于基材的方向上的扩散率从低于 ∼10–17cm2s–1 到 ∼10–14cm2s–1 的值变化。在胶片组装过程中。最具扩散性的 P3HMA 的吸收表现出亚扩散行为，异常扩散指数 β ≈ 0.3。同样，中子反射法揭示了薄膜动力学的巨大差异，中子反射法检测到氘代 PEO (dPEO) 快速渗透整个薄膜，其扩散系数 >10-12cm2s-1 通过 P3HMA/PEO 薄膜，但在暴露于 dPEO 的前 10 分钟内，所有其他 lPPh/PEO 系统仅在薄膜表面积累 dPEO。观察到的薄膜动力学趋势与 P3HMA/PEO 薄膜的强指数增长和非扩散 P2/PEO 系统的线性沉积一致。最后，通过原位原子力显微镜实验量化了 IPPh/PEO 薄膜在水性环境中的自修复行为，结果表明 P3/PEO 薄膜在几分钟的时间内发生了强大的自修复作用，而 P2/PEO 薄膜则没有薄膜愈合。
This work explores the dynamics of hydrogen-bonded layer-by-layer (LbL) films of linear synthetic polyphenols (lPPh’s) with different backbone and pendant group structures. The polymers feature repeat units with catechol-like or gallol-like polyphenol rings, namely, poly(3,4-dihydroxybenzyl methacrylamide) (P2HMA), poly(3,4-dihydroxybenzyl acrylamide) (P2HAA), poly(3,4,5-trihydroxybenzyl acrylamide) (P3HAA), and poly(3,4,5-trihydroxybenzyl methacrylamide) (P3HMA), and were assembled with linear poly(ethylene oxide) (PEO). The structure of thelPPh’s has a major effect on the diffusivity of LbL films, and chain dynamics is asymmetric forlPPh- and PEO-terminated films during film construction.Specifically, diffusivity of polyphenols in the direction perpendicular to the substrate varied from values below ∼10–17cm2s–1to ∼10–14cm2s–1forlPPh’s of the P2 and P3 families, as assessed byin situellipsometry during film assembly. The uptake of the most diffusive P3HMA exhibits subdiffusive behavior with an anomalous diffusion exponent β ≈ 0.3. Similarly, large differences in film dynamics were revealed by neutron reflectometry, which detected fast penetration of deuterated PEO (dPEO) through the entire film with a diffusion coefficient >10–12cm2s–1through P3HMA/PEO films but accumulation ofdPEO only at the film surface for all otherlPPh/PEO systems during the first 10 min of exposure todPEO. The observed trends in film dynamics were consistent with strongly exponential growth of P3HMA/PEO films and largely linear deposition of nondiffusive P2/PEO systems. Finally, the self-healing behavior oflPPh/PEO films in an aqueous environment was quantified byin situatomic force microscopy experiments, which revealed robust self-healing of P3/PEO films occurring on a time scale of minutes and an absence of film healing for P2/PEO films.
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影响因子：
7.015
作者：
Xu L;Kozlovskaya V;Kharlampieva E;Ankner JF;Sukhishvili SA
通讯作者：
Sukhishvili SA
pH 诱导的聚阴离子从多层膜中释放。
影响因子：
8.6
作者：
E. Kharlampieva;J. Ankner;M. Rubinstein;S. Sukhishvili
通讯作者：
S. Sukhishvili
影响因子：
5.5
作者：
Hlushko, Raman;Ankner, John F.;Sukhishvili, Svetlana A.
通讯作者：
Sukhishvili, Svetlana A.
影响因子：
14
作者：
Pham-Hua D;Padgett LE;Xue B;Anderson B;Zeiger M;Barra JM;Bethea M;Hunter CS;Kozlovskaya V;Kharlampieva E;Tse HM
通讯作者：
Tse HM
影响因子：
5.5
作者：
Soltwedel, Olaf;Ivanova, Oxana;Helm, Christiane A.
通讯作者：
Helm, Christiane A.