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用氧化还原水凝胶修饰碳纳米管:提高氧化还原酶的安培传感灵敏度。

Modification of carbon nanotubes with redox hydrogel: improvement of amperometric sensing sensitivity for redox enzymes.

作者信息

Cui Hui-Fang, Ye Jian-Shan, Zhang Wei-De, Sheu Fwu-Shan

机构信息

Department of Bioengineering, Zhengzhou University, Zhengzhou, PR China.

出版信息

Biosens Bioelectron. 2009 Feb 15;24(6):1723-9. doi: 10.1016/j.bios.2008.09.002. Epub 2008 Sep 12.

Abstract

This study demonstrated that redox hydrogel-modified carbon nanotube (CNT) electrodes can be developed as an amperometric sensor that are sensitive, specific and fast and do not require auxiliary enzymes. A redox polymer, poly(vinylimidazole) complexed with Os(4,4'-dimethylbpy)(2)Cl (PVI-dmeOs) was electrodeposited on Ta-supported multi-walled CNTs. The resulted PVI-dmeOs thin film did not change the surface morphology of the CNTs, but turned the CNT surface from hydrophobic to hydrophilic, as studied by scanning electron microscopy (SEM) and static water contact angle measurements. Cyclic voltammetry measurements in a Fe(CN)(6)(3-) solution and electrochemical impedance measurements in an equimolar Fe(CN)(6)(3-/4-) solution demonstrated that the PVI-dmeOs hydrogel thin film was electronic conductive with a resistance of about 15Omega. The PVI-dmeOs/CNT electrodes sensed rapidly, sensitively and specifically to model redox enzymes (glucose oxidase (GOD) and lactate oxidase (LOD)) in amperometric experiments in electrolyte solutions containing the substrates of the measured redox enzymes. Both the CNT substrate and the thin PVI-dmeOs film enhanced the sensing sensitivities. Exploration of the mechanisms suggests that the PVI-dmeOs film may enhance the sensing sensitivities by wiring the enzyme molecules through the redox centers tethered on the mobile redox polymer backbones to the CNT electrodes.

摘要

本研究表明,氧化还原水凝胶修饰的碳纳米管(CNT)电极可被开发为一种电流型传感器,该传感器灵敏、特异、快速且无需辅助酶。一种与Os(4,4'-二甲基联吡啶)(2)Cl络合的氧化还原聚合物聚(乙烯基咪唑)(PVI-dmeOs)被电沉积在钽负载的多壁碳纳米管上。通过扫描电子显微镜(SEM)和静态水接触角测量研究发现,所得的PVI-dmeOs薄膜并未改变碳纳米管的表面形态,但将碳纳米管表面由疏水变为亲水。在Fe(CN)(6)(3-)溶液中的循环伏安测量以及在等摩尔Fe(CN)(6)(3-/4-)溶液中的电化学阻抗测量表明,PVI-dmeOs水凝胶薄膜具有电子导电性,电阻约为15Ω。在含有被测氧化还原酶底物的电解质溶液的电流实验中,PVI-dmeOs/CNT电极对模型氧化还原酶(葡萄糖氧化酶(GOD)和乳酸氧化酶(LOD))具有快速、灵敏且特异的传感性能。碳纳米管基底和PVI-dmeOs薄膜均提高了传感灵敏度。对其作用机制的探究表明,PVI-dmeOs薄膜可能通过将酶分子通过连接在可移动氧化还原聚合物主链上的氧化还原中心连接到碳纳米管电极来提高传感灵敏度。

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