Strong interaction between imidazolium-based polycationic polymer and ferricyanide: toward redox potential regulation for selective in vivo electrochemical measurements.
Strong interaction between imidazolium-based polycationic polymer and ferricyanide: toward redox potential regulation for selective in vivo electrochemical measurements.
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DOI：
10.1021/ac202748s
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发表时间：
2012-02
影响因子：
7.4
通讯作者：
Xuming Zhuang;Dalei Wang;Yuqing Lin;Lifen Yang;Ping Yu;Wei Jiang;L. Mao
中科院分区：
文献类型：
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作者：
Xuming Zhuang;Dalei Wang;Yuqing Lin;Lifen Yang;Ping Yu;Wei Jiang;L. Mao
这项研究有效地展示了一种策略，使基于铁氰化铁的第二代生物传感器能够选择性地在体内测量神经化学物质，并以葡萄糖为例。该策略通过仔细控制铁氰化物(Fe(CN)(6)(3-))和亚铁氰化物(Fe(CN)(6)(4-))在电极表面的不同吸附能力来调节铁氰化物介体的氧化还原电位。为了实现Fe(CN)(6)(3-/4-)氧化还原电位的负移，合成了咪唑基聚合物(Pim)，由于其与Fe(CN)(6)(3-)的相互作用比与Fe(CN)(6)(4-)的作用更强，因此被用作Fe(CN)(6)(3-/4-)表面吸附的基质。Fe(CN)(6)(3-)和Fe(CN)(6)(4-)在PIM和多壁碳纳米管(MWNTs)复合修饰电极上的不同吸附能力最终使这两种物种稳定的表面吸附形成集成的生物传感器，更重要的是，导致表面受限的氧化还原介体的氧化还原电位负移。以葡萄糖氧化酶(GOD)为模型生物识别单元，我们证明了基于铁氰化物的第二代生物传感器在体内选择性神经化学测量中的有效性。我们发现，根据本研究中所展示的策略开发的生物传感器，通过与体内微透析相结合，可以很好地作为连续在线检测豚鼠纹状体葡萄糖的选择性检测器。这项研究基本上为开发有效用于体内神经化学测量的电化学生物传感器铺平了一条新的途径，这对于理解生理和病理事件的分子基础具有重要意义。
This study effectively demonstrates a strategy to enable the ferricyanide-based second-generation biosensors for selective in vivo measurements of neurochemicals, with glucose as an example. The strategy is based on regulation of redox potential of ferricyanide mediator by carefully controlling the different adsorption ability of ferricyanide (Fe(CN)(6)(3-)) and ferrocyanide (Fe(CN)(6)(4-)) onto electrode surface. To realize the negative shift of the redox potential of Fe(CN)(6)(3-/4-), imidazolium-based polymer (Pim) is synthesized and used as a matrix for surface adsorption of Fe(CN)(6)(3-/4-) due to its stronger interaction with Fe(CN)(6)(3-) than with Fe(CN)(6)(4-). The different adsorption ability of Fe(CN)(6)(3-) and Fe(CN)(6)(4-) onto electrodes modified with a composite of Pim and multiwalled carbon nanotubes (MWNTs) eventually enables the stable surface adsorption of both species to generate integrated biosensors and, more importantly, leads to a negative shift of the redox potential of the surface-confined redox mediator. Using glucose oxidase (GOD) as the model biorecognition units, we demonstrate the validity of the ferricyanide-based second-generation biosensors for selective in vivo neurochemical measurements. We find that the biosensors developed with the strategy demonstrated in this study can be used well as the selective detector for continuous online detection of striatum glucose of guinea pigs, by integration with in vivo microdialysis. This study essentially paves a new avenue to developing electrochemical biosensors effectively for in vivo neurochemical measurements, which is envisaged to be of great importance in understanding the molecular basis of physiological and pathological events.