pH-, Sugar-, and Temperature-Sensitive Electrochemical Switch Amplified by Enzymatic Reaction and Controlled by Logic Gates Based on Semi-Interpenetrating Polymer Networks
pH-, Sugar-, and Temperature-Sensitive Electrochemical Switch Amplified by Enzymatic Reaction and Controlled by Logic Gates Based on Semi-Interpenetrating Polymer Networks
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基于半互穿聚合物网络的酶反应放大并由逻辑门控制的 pH、糖和温度敏感电化学开关
DOI：
10.1021/jp209788g
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发表时间：
2012-02-09
影响因子：
3.3
通讯作者：
Hu, Naifei
中科院分区：
文献类型：
--
作者：
Liu, Dan;Liu, Hongyun;Hu, Naifei
将苯基硼酸（PBA）接枝到聚丙烯酸（PAA）的主链上，形成PAA-PBA嵌段共聚物。然后在电极表面制备了聚N，N-二乙基丙烯酰胺（PDEA）与聚丙烯酸-聚丙烯酸丁酯（PAA-PBA）的半互穿聚合物网络（semi-IPN）膜，并包埋辣根过氧化物酶（HRP），命名为PDEA-（PAA-PBA）-HRP。该膜在循环伏安（CV）响应中表现出对电活性探针K3 Fe（CN）（6）可逆的pH-、果糖-和热响应的开-关行为。该体系的多开关CV行为可进一步用于控制和调节固定在膜中的HRP以K3 Fe（CN）（6）为介体在溶液中催化H2 O2的电化学还原。并对系统的响应机理进行了探讨。pH敏感性归因于膜中PAA组分与探针在不同pH下的静电相互作用;温度响应性归因于膜中PDEA水凝胶组分的结构随温度的变化;果糖敏感性归因于膜中PBA组分与糖的络合作用引起的膜结构变化。这种智能系统可以作为一个3输入逻辑网络组成的启用或（EnOR）门在化学或生物分子计算相结合的多响应特性和生物电催化的放大效应，并展示了潜在的前景，制造新型的多开关电化学生物传感器和生物电子器件。
Phenylboronic acid (PBA) moieties are grafted onto the backbone of poly(acrylic acid) (PAA), forming the PAA-PBA polyelectrolyte. The semi-interpenetrating polymer network (semi-IPN) films composed of PAA-PBA and poly(N,N-diethylacrylamide) (PDEA) were then synthesized on electrode surface with entrapped horseradish peroxidase (HRP), designated as PDEA-(PAA-PBA)-HRP. The films demonstrated reversible pH-, fructose-, and thermo-responsive on-off behavior toward electroactive probe K3Fe(CN)(6) in its cyclic voltammetric (CV) response. This multiswitchable CV behavior of the system could be further employed to control and modulate the electrochemical reduction of H2O2 catalyzed by HRP immobilized in the films with K3Fe(CN)(6) as the mediator in solution. The responsive mechanism of the system was also explored and discussed. The pH-sensitive property was attributed to the electrostatic interaction between the PAA component of the films and the probe at different pH; the thermo-responsive behavior originated from the structure change of PDEA hydrogel component of the films with temperature; the fructose-sensitive property was ascribed to the structure change of the films induced by the complexation between the PBA constituent and the sugar. This smart system could be used as a 3-input logic network composed of enabled OR (EnOR) gates in chemical or biomolecular computing by combining the multiresponsive property of the films and the amplification effect of bioelectrocatalysis and demonstrated the potential perspective for fabricating novel multiswitchable electrochemical biosensors and bioelectronic devices.