Tailoring 1,4-naphthoquinone with electron-withdrawing group: toward developing redox polymer and FAD-GDH based hydrogel bioanode for efficient electrocatalytic glucose oxidation

Tailoring 1,4-naphthoquinone with electron-withdrawing group: toward developing redox polymer and FAD-GDH based hydrogel bioanode for efficient electrocatalytic glucose oxidation
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用吸电子基团定制 1,4-萘醌:开发氧化还原聚合物和基于 FAD-GDH 的水凝胶生物阳极,用于高效电催化葡萄糖氧化

DOI:
10.1016/j.electacta.2016.06.078
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发表时间:
2016-09-01
影响因子:
6.6
通讯作者:
Liu, Aihua
Liu, Aihua
中科院分区:
材料科学2区
文献类型:
--
作者:
Hou, Chuantao;Lang, Qiaolin;Liu, Aihua

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氧化还原聚合物水凝胶在生物燃料电池设计和电化学生物传感方面具有广阔的应用前景。本文报道了一种基于吸电子硝基修饰的1,4-萘醌(1,4-NQ)修饰的氧化还原聚合物和黄素腺嘌呤二核苷酸依赖性葡萄糖脱氢酶(FAD-GDH)的水凝胶生物阳极可以显著提高葡萄糖氧化的催化性能,在50 mM葡萄糖溶液中,不使用任何纳米材料作为电极支撑物,可以获得1.97 ± 0.06 mA cm(-2)的高电流密度和-0.13 V(vs. Ag/AgCl)的低起始电位。此外,还合成了供电子基团修饰的1,4-硝基喹啉和吸电子硝基修饰的1,4-硝基喹啉,并对其电化学性能进行了研究。结果表明,硝基修饰的1,4-NQs修饰的氧化还原聚合物使葡萄糖氧化的形式电位正移,为葡萄糖氧化提供了足够的电化学驱动力,从而提高了催化剂的催化性能.最后,将该水凝胶阳极与胆红素氧化酶生物阴极相结合,构建了单室葡萄糖/O-2生物燃料电池,其输出功率为0.28 ± 0.03 mW cm(-2),开路电位为0.69 V。该研究为开发直接从葡萄糖中获取能量的葡萄糖生物传感器或生物燃料电池提供了一种替代途径。(C)2016爱思唯尔有限公司版权所有
Redox polymer hydrogels have been proved to be very promising for biofuel cells design and electrochemical biosensing. Here we report that a facile hydrogel bioanode based on electron-withdrawing nitro-group tailored 1,4-naphthoquinone (1,4-NQ)-appended redox polymer and flavin adenine dinucleotide-dependent glucose dehydrogenase (FAD-GDH) can dramatically improve the catalytic performance of glucose oxidation, for which a high current density of 1.97 + 0.06 mA cm(-2) and low onset potential of -0.13 V (vs. Ag/AgCl) can be achieved in 50 mM glucose solution without using any nanomaterials as electrode supports. Further, both electron-donating groups modified 1,4-NQs and electron-withdrawing nitro-group 1,4-NQs were synthesized to investigate their electrochemical properties. It was found that the enhanced catalytic performance can be mainly contributing from the nitro group-modified 1,4-NQs appended redox polymer, which shifted the formal potential in the positive direction and provided sufficient electrochemical driving force for glucose oxidation. Finally, this hydrogel bioanode was combined with a bilirubin oxidase based biocathode to construct a single-compartment glucose/O-2 biofuel cell with a high power output of 0.28 +/- 0.03 mW cm(-2) and open circuit potential of 0.69 V. Moreover, the O-2-insensitive FAD-GDH could improve the cell stability obviously compared with glucose oxidase based cell. This study provides an alternative route to develop glucose biosensor or biofuel cell for directly harvesting energy from glucose. (C) 2016 Elsevier Ltd. All rights reserved.