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Functionalized carbon nanotube adsorption interfaces for electron transfer studies of galactose oxidase
Bioelectrochemistry ( IF 5 ) Pub Date : 2018-10-19 , DOI: 10.1016/j.bioelechem.2018.10.003
Mulugeta B. Wayu , Michael J. Pannell , Najwa Labban , William S. Case , Julie A. Pollock , Michael C. Leopold

Modified electrodes featuring specific adsorption platforms able to access the electrochemistry of the copper containing enzyme galactose oxidase (GaOx) were explored, including interfaces featuring nanomaterials such as nanoparticles and carbon nanotubes (CNTs). Electrodes modified with various self-assembled monolayers (SAMs) including those with attached nanoparticles or amide-coupled functionalized CNTs were examined for their ability to effectively immobilize GaOx and study the redox activity related to its copper core. While stable GaOx electrochemistry has been notoriously difficult to achieve at modified electrodes, strategically designed functionalized CNT-based interfaces, cysteamine SAM-modified electrode subsequently amide-coupled to carboxylic acid functionalized single wall CNTs, were significantly more effective with high GaOx surface adsorption along with well-defined, more reversible, stable (≥ 8 days) voltammetry and an average ET rate constant of 0.74 s−1 in spite of increased ET distance - a result attributed to effective electronic coupling at the GaOx active site. Both amperometric and fluorescence assay results suggest embedded GaOx remains active. Fundamental ET properties of GaOx may be relevant to biosensor development targeting galactosemia while the use functionalized CNT platforms for adsorption/electrochemistry of electroactive enzymes/proteins may present an approach for fundamental protein electrochemistry and their future use in both direct and indirect biosensor schemes.



中文翻译:

功能化碳纳米管吸附界面,用于半乳糖氧化酶的电子转移研究

探索了具有特定吸附平台的修饰电极,该特定吸附平台能够访问含铜酶半乳糖氧化酶(GaOx)的电化学,包括具有纳米材料(例如纳米粒子和碳纳米管(CNT))的界面。研究了用各种自组装单分子膜(SAMs)修饰的电极,包括与纳米颗粒或酰胺偶联的官能化CNT连接的电极的有效固定GaOx的能力,并研究了与其铜核有关的氧化还原活性。尽管众所周知,在修饰电极上难以实现稳定的GaOx电化学,但在战略上设计了功能化的基于CNT的界面,半胱胺SAM修饰的电极随后通过酰胺偶联到了羧酸官能化的单壁CNT上,尽管ET距离增加,但-1-这归因于GaOx活性位点处的有效电子耦合。安培和荧光测定结果均表明,嵌入的GaOx仍保持活性。GaOx的基本ET特性可能与针对半乳糖血症的生物传感器开发有关,而将功能化CNT平台用于电活性酶/蛋白质的吸附/电化学可为基本蛋白质电化学及其在直接和间接生物传感器计划中的未来应用提供一种方法。

更新日期:2018-10-19
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