Coupling Self-Assembly Mechanisms to Fabricate Molecularly and Electrically Responsive Films
Coupling Self-Assembly Mechanisms to Fabricate Molecularly and Electrically Responsive Films
复制标题
耦合自组装机制来制造分子和电响应薄膜
DOI：
10.1021/acs.biomac.8b01592
复制
发表时间：
2019-02-01
影响因子：
6.2
通讯作者：
Payne, Gregory F.
中科院分区：
文献类型：
--
作者：
Li, Jinyang;Maniar, Drishti;Payne, Gregory F.
生物大分子通常具有通过低能量竞争相互作用进行自组装的信息，这种相互作用可以使自组装响应环境信号并赋予动态特性。在这里，我们将自组装系统耦合在一起，创造出具有生物功能的多层膜，这种膜可以通过分子或电信号来引导分解。为了创建功能多层，我们：(i)电沉积ph响应自组装氨基多糖壳聚糖，（ii）允许凝集素ConA （ConA）结合到壳聚糖包覆的电极上（可能是通过静电相互作用），（iii）通过与糖原和ConA的顺序接触进行逐层自组装，以及（iv）通过将糖蛋白（即酶）组装到ConA端终止的多层上，赋予生物（即酶）功能。由于ConA四聚体在低pH下解离，该多层膜可以通过酸化触发分解。我们展示了两种诱导酸化的方法：(i)葡萄糖氧化酶可以根据分子信号诱导多层分解，（ii）阳极反应可以根据电信号诱导多层分解。
Biomacromolecules often possess information to self-assemble through low energy competing interactions which can make self-assembly responsive to environmental cues and can also confer dynamic properties. Here, we coupled self-assembling systems to create biofunctional multilayer films that can be cued to disassemble through either molecular or electrical signals. To create functional multilayers, we: (i) electrodeposited the pH-responsive self-assembling amino-polysaccharide chitosan, (ii) allowed the lectin Concanavalin A (ConA) to bind to the chitosan-coated electrode (presumably through electrostatic interactions), (iii) performed layer-by-layer self-assembly by sequential contacting with glycogen and ConA, and (iv) conferred biological (i.e., enzymatic) function by assembling glycoprotein (i.e., enzymes) to the ConA-terminated multilayer. Because the ConA tetramer dissociates at low pH, this multilayer can be triggered to disassemble by acidification. We demonstrate two approaches to induce acidification: (i) glucose oxidase can induce multilayer disassembly in response to molecular cues, and (ii) anodic reactions can induce multilayer disassembly in response to electrical cues.