金纳米粒子-壳聚糖-石墨烯纳米复合材料的制备及其在生物电化学中的应用

doi:10.6023/A12060284

化学学报 ›› 2012, Vol. 70 ›› Issue (21): 2213-2219.DOI: 10.6023/A12060284 上一篇下一篇

研究论文

金纳米粒子-壳聚糖-石墨烯纳米复合材料的制备及其在生物电化学中的应用

张谦^a,b, 吴抒遥^a,b, 何茂伟^a,b, 张玲^c, 刘洋^d, 李景虹^d, 宋溪明^a,b

a 辽宁大学绿色合成与先进材料制备化学辽宁省重点实验室沈阳 110036;
b 辽宁大学化学院沈阳 110036;
c 沈阳师范大学化学与生命科学学院沈阳 110034;
d 清华大学化学系北京 100084

投稿日期:2012-06-06 发布日期:2012-09-17
通讯作者: 李景虹, 宋溪明 E-mail:songlab@lnu.edu.cn, jhli@mail.tsinghua.edu.cn
基金资助:
项目受国家自然科学基金(Nos. 21071070, 21005046, 20901035, 51273087, 21235004, 21203126)、辽宁省高等学校创新团队基金(No. LT2011001)、辽宁省自然科学基金(No. 201202088)、2013年辽宁大学青年科研基金和辽宁大学创新人才培养基金资助.

Preparation and Bioelectrochemical Application of Gold Nanoparticles-Chitosan-Graphene Nanomaterials

Zhang Qian^a,b, Wu Shuyao^a,b, He Maowei^a,b, Zhang Ling^c, Liu Yang^d, Li Jinghong^d, Song Xi-Ming^a,b

a Liaoning Provincial Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials, Liaoning University, Shenyang 110036;
b College of Chemistry, Liaoning University, Shenyang 110036;
c College of Chemistry and Life Science, Shenyang Normal University, Shenyang 110034;
d Department of Chemistry, Tsinghua University, Beijing 100084

Received:2012-06-06 Published:2012-09-17
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 21071070, 21005046, 20901035, 51273087, 21235004 and 21203126), the Program for Liaoning Innovative Research Team in University (No. LT2011001), Natural Science Foundation of Liaoning Province (No. 201202088), the Foundation for Young Scholars of Liaoning University (2013) and the Foundation of 211 Project for Innovative Talents Training, Liaoning University.

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摘要/Abstract

通过共价键作用和原位还原法制备了金纳米粒子/壳聚糖-石墨烯纳米复合材料(AuNPs/Chit-GP). 利用FT-IR, UV-vis, TEM以及XRD对所合成的纳米复合物的结构和形貌进行了表征. AuNPs/Chit-GP呈现明显的正电荷, 因此可通过静电相互作用固载葡萄糖氧化酶(GOD), 并构建GOD/AuNPs/Chit-GP/GC修饰电极. 该修饰电极不仅可成功地实现GOD与电极间的直接电子转移, 还对葡萄糖表现出良好的催化性能. 实验结果表明, 其催化的线性范围为2.1～5.7 μmol/L, 检出限为0.7 μmol/L, 灵敏度为79.71 mA·cm^-2·mM^-1. 这种集金属纳米粒子、生物相容性高分子以及石墨烯为一体的纳米复合物的构筑为无媒介体的电化学生物传感器的研究提供了一个良好的平台.

关键词: 纳米金, 壳聚糖, 石墨烯, 葡萄糖氧化酶, 直接电化学

Based on the covalent modification and in-situ reduction, chitosan and gold nanoparticles were integrated with graphene to form a novel gold nanoparticles/chitosan-graphene (AuNPs/Chit-GP) nanocomposite. The process of the fabrication of AuNPs/Chit-GP nanocomposite consisted of the following steps. Firstly, carboxyl-GP was prepared based on the reduction and modification of graphene oxide (GO). Thereafter, chitosan was covalently functionalized onto graphene nanosheet to fabricate Chit-GP. The AuNPs/Chit-GP nanocomposite was finally synthesized by the in-situ reduction of HAuCl₄in the presence of Chit-GP. Fourier transform infrared (FT-IR) spectra, ultraviolet-visible (UV-vis) absorption spectra, transmission electron microscopy (TEM) and X-ray diffraction (XRD) were utilized to characterize structure and morphology of the as synthesized nanocomposite. Because of the surface functionalization of chitosan, the composite exhibited positive charge. In that case, the negatively charged glucose oxidase (GOD) could further immobilize onto AuNPs/Chit-GP via electrostatic interaction under mild experimental condition. With the advantages of graphene, Au nanoparticles and chitosan, AuNPs/Chit-GP can offer a conductive and favorable microenvironment for the immobilized GOD to achieve direct electrochemistry. The direct electron transfer (DET) reaction of the immoblized GOD was studied by cyclic voltammetry in 0.1 mol/L phosphate buffer solution (PBS, pH 7.4). A pair of well-defined, quasi-reversible redox peaks of GOD were obtained at GOD/AuNPs/Chit-GP/GC modified electrode, with a formal potential (vs. Ag/AgCl) being -0.44 V. Moreover, the as fabricated GOD/AuNPs/Chit-GP/GC modified electrode exhibited excellent catalytic performance towards glucose. The electrocatalytic response of GOD/AuNPs/Chit-GP/GC modified electrode altered linearly with the glucose concentration ranging from 2.1 to 5.7 μmol/L. The detection limit and the sensitivity of the enzyme electrode were 0.7 μmol/L (S/N＝3) and 79.71 mA·cm^-2·mM^-1, respectively. Because of the biocompability of the AuNPs/Chit-GP, GOD/AuNPs/Chit-GP/GC modified electrode also exhibited acceptable reproducibility and excellent stability. Therefore, such a novel nanocomposite composed of metal nanoparticles, biocompatible macromolecules and graphene provides an efficient platform for the development of mediator-free electrochemical biosensors.

Key words: gold nanoparticles, chitosan, graphene, glucose oxidase, direct electrochemistry

引用此文

张谦, 吴抒遥, 何茂伟, 张玲, 刘洋, 李景虹, 宋溪明. 金纳米粒子-壳聚糖-石墨烯纳米复合材料的制备及其在生物电化学中的应用[J]. 化学学报, 2012, 70(21): 2213-2219.

Zhang Qian, Wu Shuyao, He Maowei, Zhang Ling, Liu Yang, Li Jinghong, Song Xi-Ming. Preparation and Bioelectrochemical Application of Gold Nanoparticles-Chitosan-Graphene Nanomaterials[J]. Acta Chimica Sinica, 2012, 70(21): 2213-2219.

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金纳米粒子-壳聚糖-石墨烯纳米复合材料的制备及其在生物电化学中的应用

Preparation and Bioelectrochemical Application of Gold Nanoparticles-Chitosan-Graphene Nanomaterials

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