Xiang Ling, Zhang Zhinan, Yu Ping, Zhang Jun, Su Lei, Ohsaka Takeo, Mao Lanqun
Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, the Chinese Academy of Sciences (CAS), Beijing 100080, China.
Anal Chem. 2008 Sep 1;80(17):6587-93. doi: 10.1021/ac800733t. Epub 2008 Aug 1.
This study demonstrates a new and relatively general route to the development of multiwalled carbon nanotube (MWNT)-based integrative electrochemical biosensors by confining ferricyanide redox mediator onto MWNTs. The ferricyanide-confined MWNTs are synthesized first through grafting of epoxy chloropropane onto MWNTs with in situ cationic ring-opening polymerization and then introducing the positively charged methylimidazolium moieties into the grafted polymer with a quaternization reaction. The grafted polymers with positively charged methylimidazolium moieties tethered onto MWNTs can essentially be used to confine redox-active ferricyanide onto MWNTs to form a redox mediator-confined nanocomposite with a good stability and excellent electrochemical property. The synthetic nanocomposite with surface-confined ferricyanide is demonstrated to be well-competent as the efficient electronic transducers for the general development of electrochemical biosensors upon combination with biorecognition units, which is illustrated by using glucose oxidase and laccase as two model biorecognition units. This study essentially paves a facile and general approach to the development of integrative nanostructured electrochemical biosensors.
本研究展示了一种通过将铁氰化物氧化还原介质限制在多壁碳纳米管(MWNT)上,来开发基于MWNT的集成电化学生物传感器的新的且相对通用的途径。首先通过环氧氯丙烷在MWNT上的接枝以及原位阳离子开环聚合反应,合成出铁氰化物限制的MWNT,然后通过季铵化反应将带正电荷的甲基咪唑基团引入接枝聚合物中。带有带正电荷甲基咪唑基团的接枝聚合物连接在MWNT上,基本上可用于将氧化还原活性铁氰化物限制在MWNT上,从而形成具有良好稳定性和优异电化学性能的氧化还原介质限制纳米复合材料。经证明,表面限制有铁氰化物的合成纳米复合材料,在与生物识别单元结合后,作为电化学生物传感器通用开发的高效电子换能器表现出色,以葡萄糖氧化酶和漆酶作为两个模型生物识别单元对此进行了说明。本研究实质上为集成纳米结构电化学生物传感器的开发铺平了一条简便通用的途径。