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首页> 外文期刊>Journal of Materials Chemistry, B. materials for biology and medicine >Surface self-assembled hybrid nanocomposites with electroactive nanoparticles and enzymes confined in a polymer matrix for controlled electrocatalysis
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Surface self-assembled hybrid nanocomposites with electroactive nanoparticles and enzymes confined in a polymer matrix for controlled electrocatalysis

机译：具有电活性纳米颗粒和酶的表面自组装杂化纳米复合材料，其酶被限制在聚合物基质中以控制电催化作用

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摘要

A three-dimensional network of highly branched poly(ethyleneimine) (PEI) is designed and synthesized on gold electrode surfaces. A self-assembled monolayer (SAM) of dithiobis(succinimidyl propionate) (DTSP) on a gold electrode was first prepared, which is confirmed by the reductive desorption of Au-S units. The PEI polymer was then covalently immobilized onto the DTSP layer, leaving free primary amine groups acting as a 3D skeleton for high loading of electroactive enzyme-size Prussian blue nanoparticles (PBNPs, 6 nm) via electrostatic trapping. Atomic force microscopy was used to disclose the microscopic structures of the different layers during the surface architecture formation. The resulting surface-bound nanostructured composite shows high electrochemical activity arising from confined PBNPs, and acts as an efficient electrocatalyst towards H2O2 reduction. Facile electron communication is achieved as reflected by a large electron transfer (ET) rate constant (k(s)) of 200 s(-1), and the possible electron propagation mechanisms in the polymer network are discussed. This surface/interfacial nanocomposite can be further used in the accommodation of enzymes for electrochemical bio-catalysis. Glucose oxidase (GOD) was used towards this end, in a proof-of-concept study. This enzyme can be co-trapped in the PEI matrix and is interconnected with PBNPs, leading to highly efficient electrocatalyic oxidation and detection of glucose.
机译：设计并在金电极表面合成了高度支化的聚亚乙基亚胺（PEI）三维网络。首先在金电极上制备了自组装的二硫代双（琥珀酰亚胺丙酸酯）（DTSP）单分子膜（SAM），这通过Au-S单元的还原脱附得到证实。然后将PEI聚合物共价固定在DTSP层上，留下游离的伯胺基团作为3D骨架，以通过静电捕获高负载电活性酶大小的普鲁士蓝纳米颗粒（PBNPs，6 nm）。原子力显微镜用于揭示表面结构形成过程中不同层的微观结构。所得的表面结合的纳米结构复合材料显示出由受限的PBNP引起的高电化学活性，并充当有效的H2O2还原电催化剂。通过200 s（-1）的大电子传输（ET）速率常数（k（s））可以实现轻松的电子通信，并讨论了聚合物网络中可能的电子传播机理。该表面/界面纳米复合材料可进一步用于酶的容纳以进行电化学生物催化。为此，在概念验证研究中使用了葡萄糖氧化酶（GOD）。该酶可以共捕获在PEI基质中，并与PBNP互连，从而导致高效的电催化氧化和葡萄糖检测。

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