Electrochemically Controlled Adsorption of Fc-Functionalized Polymers on β-CD-Modified Self-Assembled Monolayers
Electrochemically Controlled Adsorption of Fc-Functionalized Polymers on β-CD-Modified Self-Assembled Monolayers
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DOI：
10.1021/la102026h
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发表时间：
2010-09-07
期刊：
影响因子：
3.9
通讯作者：
Labbe, Pierre
中科院分区：
文献类型：
--
作者：
Dubacheva, Galina V.;Van der Heyden, Angeline;Labbe, Pierre
研究了二茂铁(FC)功能化的线型聚合物在β-环糊精(β-CD)修饰的自组装单分子膜(SAM)表面的吸附/脱附行为。用石英晶体微天平结合耗散监测(QCM-D)、循环伏安和接触角测量对HS-(CH2)(11)-EG(6)-N-3和HS-(CH2)(11)-EG(4)-OH(EG，乙二醇)的二元自组装膜进行了表征。通过SAMS显示的β-CD单炔基衍生物与叠氮基之间的“点击”反应，实现了SAMS与β-CD的功能化。用QCM-D研究了SAM-β-CD与FC衍生聚合物(壳聚糖(CHI)和聚烯丙胺盐酸盐(PAH))之间的主客体络合物的形成。用Voinova粘弹性模型拟合了CHI-FC和PAH-FC在SAM-β-CD上的吸附和电化学控制脱附过程中的QCM-D曲线。利用QCM-D与循环伏安相结合的方法，我们证明了CHI-FC和PAH-FC可以成功地沉积在SAM-β-CD包覆的金表面上，在聚合物的Fe部分与SAM的β-CD空腔之间形成稳定的多价包合物。我们还表明，在外加电场的作用下，所有特定连接的高分子链都可以从SAM-β-CD涂层的金表面上分离出来。
This work presents an in situ study of the adsorption/desorption behavior of ferrocene(Fc)-functionalized linear polymers on a gold surface covered with beta-cyclodextrin(beta-CD)-modified self-assembled monolayers (SAMs). The characterization of binary SAMs obtained with HS-(CH2)(11)-EG(6)-N-3 and HS-(CH2)(11)-EG(4)-OH (EG, ethylene glycol) was performed using a quartz crystal microbalance with dissipation monitoring (QCM-D), cyclic voltammetry, and contact angle measurements. The functionalization of SA Ms with beta-CD was made via the "click" reaction between the beta-CD monoalkyne derivative and azide groups exhibited by SA Ms. The formation of the host-guest complex between SAM-beta-CD and Fc-derivatized polymers (chitosan (CHI) and poly(allylamine hydrochloride) (PAH)) was studied by QCM-D. The viscoelastic model of Voinova was used to fit QCM-D curves recorded during the adsorption and electrochemically controlled desorption of CHI-Fc and PAH-Fc on SAM-beta-CD. Using QCM-D coupled to cyclic voltammetry, we demonstrated that CHI-Fc and PAH-Fc can be successfully deposited on a SAM-beta-CD-coated gold surface forming a stable multivalent inclusion complex between Fe moieties of polymer and beta-CD cavities of SAM. We also showed that all specifically attached polymer chains can be detached from the SAM-beta-CD-coated gold surface by applying an electric field.