基于碳纳米管和铂纳米粒子的葡萄糖电化学生物传感器
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摘要
电化学传感器是检测葡萄糖水平的有效手段,开发新的电极表面修饰材料以提高电极灵敏度和延长使用寿命成为研究者关注的一个重要方面。纳米材料以其独特的电学性质被用以提高电极灵敏度,其中,碳纳米管和以铂、金、银为主的贵金属纳米材尤为应用广泛。在此背景下,本文开展了如下工作:
1.提出了一种快速、简便从而能够在传感器上批量修饰纳米材料的原位化学还原法,并将此方法成功应用于在玻璃片上修饰铂纳米颗粒。首先利用直径为10nm左右的金纳米微粒作为种子喷洒在玻璃片上,再将玻璃片浸泡到氯铂酸溶液中制备铂纳米颗粒层,最后葡萄糖氧化酶被电沉积到最外层。由这种方法制备的电极表现出优越的生物传感性能。
2.提出了一种在玻碳电极上利用种子法制备纳米颗粒的方法。先将直径约3.5nm的金颗粒与碳纳米管吸附到电极表面,再将电极浸泡到氯铂酸溶液中还原制得铂纳米颗粒层。葡萄糖氧化酶被电沉积到电极最外层表面从而制得葡萄糖电化学传感器。以该方法制得酶电极表现优越的性能,包括高灵敏度(4.49μA·mM-1),快速的反应时间(2s),低检测限(0.5μM)和宽线性范围(1μM-4mM)。可用于制备各类生物酶电极,具有广泛的应用前景。
3.报道了一种新型的电流型葡萄糖传感器,通过二茂铁修饰的碳纳米管组装而成。先将碳纳米管氨基化,再利用1-乙基-3-(3-二甲基氨丙基)-碳化二亚胺(EDC)和N-羟基琥珀酰亚胺(NHS)将羧基二茂铁上的羧基与碳纳米管上的氨基交连,再用牛血清蛋白(BSA)交连法固定葡萄糖氧化酶,制成葡萄糖传感器。分别用伏安法和计时电流法表征了制得电极的电活性,其对过氧化氢的响应电流分别高于由碳纳米管和二茂铁单独修饰的电极。
Electrochemical biosensors are effective tools for detecting glucose level, to develop new materials for electrode surface modification and to enhance electrodes’sensitivity and lifetime became an important study area. Nanomaterials are used to enhance electrodes’sensitivity due to their special electrical properties; Carbon nanotubes and novel metal nanoparticles, including platinum, gold, silver, are well-used among all kinds of nanomateirals. Therefore, this research focuses on the details as follow:
(1) A fast, simple in situ chemical reductive method is reported which can mass-produce nanomaterials onto electrodes’surfaces, and this method was successfully applied to modify platinum nanoparticles onto glass slides. Gold nanoparticles with diameter around 10nm were sputtered onto a glass slide as seeds, and then the glass slide was immersed into H2PtCl4 solution to produce Pt nanoparticle layer, and finally glucose oxidase was electrodeposited onto the outmost layer. The biosensor fabricated by this method illustrated outstanding features.
(2) A seed-mediated method was reported to grow nanoparticles onto glass carbon electrode. 3.5nm gold nanoparticles and carbon nanotubes were deposited onto electrode’s surface, and then the electrode was immersed into H2PtCl4 solution to produce Pt nanoparticles layer by reduction. Glucose oxidase was electrodeposited onto electrode’s surface to fabricate the glucose oxidase-based electrochemical biosensor. The sensor produced by this method showed excellent properties, including high sensitivity (4.49μA mM-1), fast response time (2s), low detection limit (0.5μM) and wide linear range (1μM– 4mM). This method can be used to fabricate many oxidase-based electrodes, and has wide application potential.
(3) A novel amperometric glucose sensor is reported, using ferrocene -functionalized carbon nanotubes to modify the electrodes. First amidation the carbon nanotubes, and then use 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide (EDC) and N-hydroxysuccinimide (NHS) to covalent bind the carboxyl group of ferrocene to the amino group of carbon nanotubes, and finally use bovine serum albumin (BSA) covalent binding method to immobilize the glucose oxidase onto the electrode to fabricate the sensor. Cyclic voltammograms and current-time methods were carried out to characterize the electroactivity of the proposed electrode. The results show that the response of proposed electrode toward peroxide hydrogen is higher than those of electrodes modified by simply carbon nanotubes and ferrocene respectively.
1.提出了一种快速、简便从而能够在传感器上批量修饰纳米材料的原位化学还原法,并将此方法成功应用于在玻璃片上修饰铂纳米颗粒。首先利用直径为10nm左右的金纳米微粒作为种子喷洒在玻璃片上,再将玻璃片浸泡到氯铂酸溶液中制备铂纳米颗粒层,最后葡萄糖氧化酶被电沉积到最外层。由这种方法制备的电极表现出优越的生物传感性能。
2.提出了一种在玻碳电极上利用种子法制备纳米颗粒的方法。先将直径约3.5nm的金颗粒与碳纳米管吸附到电极表面,再将电极浸泡到氯铂酸溶液中还原制得铂纳米颗粒层。葡萄糖氧化酶被电沉积到电极最外层表面从而制得葡萄糖电化学传感器。以该方法制得酶电极表现优越的性能,包括高灵敏度(4.49μA·mM-1),快速的反应时间(2s),低检测限(0.5μM)和宽线性范围(1μM-4mM)。可用于制备各类生物酶电极,具有广泛的应用前景。
3.报道了一种新型的电流型葡萄糖传感器,通过二茂铁修饰的碳纳米管组装而成。先将碳纳米管氨基化,再利用1-乙基-3-(3-二甲基氨丙基)-碳化二亚胺(EDC)和N-羟基琥珀酰亚胺(NHS)将羧基二茂铁上的羧基与碳纳米管上的氨基交连,再用牛血清蛋白(BSA)交连法固定葡萄糖氧化酶,制成葡萄糖传感器。分别用伏安法和计时电流法表征了制得电极的电活性,其对过氧化氢的响应电流分别高于由碳纳米管和二茂铁单独修饰的电极。
Electrochemical biosensors are effective tools for detecting glucose level, to develop new materials for electrode surface modification and to enhance electrodes’sensitivity and lifetime became an important study area. Nanomaterials are used to enhance electrodes’sensitivity due to their special electrical properties; Carbon nanotubes and novel metal nanoparticles, including platinum, gold, silver, are well-used among all kinds of nanomateirals. Therefore, this research focuses on the details as follow:
(1) A fast, simple in situ chemical reductive method is reported which can mass-produce nanomaterials onto electrodes’surfaces, and this method was successfully applied to modify platinum nanoparticles onto glass slides. Gold nanoparticles with diameter around 10nm were sputtered onto a glass slide as seeds, and then the glass slide was immersed into H2PtCl4 solution to produce Pt nanoparticle layer, and finally glucose oxidase was electrodeposited onto the outmost layer. The biosensor fabricated by this method illustrated outstanding features.
(2) A seed-mediated method was reported to grow nanoparticles onto glass carbon electrode. 3.5nm gold nanoparticles and carbon nanotubes were deposited onto electrode’s surface, and then the electrode was immersed into H2PtCl4 solution to produce Pt nanoparticles layer by reduction. Glucose oxidase was electrodeposited onto electrode’s surface to fabricate the glucose oxidase-based electrochemical biosensor. The sensor produced by this method showed excellent properties, including high sensitivity (4.49μA mM-1), fast response time (2s), low detection limit (0.5μM) and wide linear range (1μM– 4mM). This method can be used to fabricate many oxidase-based electrodes, and has wide application potential.
(3) A novel amperometric glucose sensor is reported, using ferrocene -functionalized carbon nanotubes to modify the electrodes. First amidation the carbon nanotubes, and then use 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide (EDC) and N-hydroxysuccinimide (NHS) to covalent bind the carboxyl group of ferrocene to the amino group of carbon nanotubes, and finally use bovine serum albumin (BSA) covalent binding method to immobilize the glucose oxidase onto the electrode to fabricate the sensor. Cyclic voltammograms and current-time methods were carried out to characterize the electroactivity of the proposed electrode. The results show that the response of proposed electrode toward peroxide hydrogen is higher than those of electrodes modified by simply carbon nanotubes and ferrocene respectively.
引文
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