磷脂修饰化的石墨烯纳米复合物的制备及其直接电化学研究

doi:10.6023/A13080911

化学学报 ›› 2014, Vol. 72 ›› Issue (3): 388-394.DOI: 10.6023/A13080911 上一篇下一篇

所属专题：石墨烯

研究论文

磷脂修饰化的石墨烯纳米复合物的制备及其直接电化学研究

张谦^a,b, 吴抒遥^a,b, 张玲^c, 茆卉^a,b, 刘大亮^a,b, 刘洋^d, 曾向群^e, 宋溪明^a,b, 李景虹^d

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;
e 奥克兰大学化学系罗切斯特市美国

投稿日期:2013-08-30 发布日期:2013-11-14
通讯作者: 李景虹，E-mail：jhli@mail.tsinghua.edu.cn；宋溪明，E-mail：songlab@lnu.edu.cn E-mail:jhli@mail.tsinghua.edu.cn；songlab@lnu.edu.cn
基金资助:
项目受国家自然科学基金（Nos. 21235004，21128005，51273087，21071070，21203126，21005046，51203072，20901035）；辽宁省高等学校创新团队基金（No. LT2011001）；辽宁省自然科学基金（Nos. 201202088，LJQ2013112）；辽宁省博士科研启动基金项目（No. 20131042）；辽宁大学青年科研基金（Nos. 2012LDQN08，2012LDQN07）；辽宁大学创新创业训练计划项目（No. X201210140036）和辽宁大学创新人才培养基金资助.

Biocompatible Phospholipid Modified Graphene Nanocomposite for Direct Electrochemistry of Redox Enzyme

Zhang Qian^a,b, Wu Shuyao^a,b, Zhang Ling^c, Mao Hui^a,b, Liu Daliang^a,b, Liu Yang^d, Zeng Xiangqun^e, Song Ximing^a,b, Li Jinghong^d

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;
e Department of Chemistry, Oakland University, Rochester USA

Received:2013-08-30 Published:2013-11-14
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 21235004, 21128005, 51273087, 21071070, 21203126, 21005046, 51203072, 20901035), the Financial Supports from the Program for Liaoning Innovative Research Team in University (No. LT2011001), the Natural Science Foundation of Liaoning Province (Nos. 201202088, LJQ2013112), the Research Fund for the Doctoral Program of Liaoning Province (No. 20131042), the Foundation for Young Scholars of Liaoning University (Nos. 2012LDQN08, 2012LDQN07), College students' innovative entrepreneurial training program (No. X201210140036) and the Foundation of 211 Project for Innovative Talents Training, Liaoning University.

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摘要/Abstract

通过非共价键修饰方法制备了兼具良好生物相容性和导电性的磷脂1-棕榈酰-2-油酰甘油-3-磷酸钠-石墨烯（POPG-GP）纳米复合物，并利用TEM，FT-IR，UV-vis，zeta电位等对其形貌和结构进行了表征. 由于POPG-GP纳米复合材料在水溶液中呈现出较为明显的负电性，因此，可通过静电自组装方法将辣根过氧化物酶（HRP）进一步组装到POPG-GP修饰的玻碳（POPG-GP/GC）电极上，构筑HRP/POPG-GP/GC修饰电极. 电化学实验结果表明，POPG-GP纳米复合物能够有效实现HRP与修饰电极之间的直接电子转移. 此外，固载在修饰电极表面的HRP对底物H₂O₂还表现出良好的电催化活性. HRP/POPG-GP/GC修饰电极对H₂O₂的检测线性范围为3.5～210 μmol/L，最低检出限为1.17 μmol/L（S/N=3），灵敏度为356.6 mA·cm^-2·M^-1，K_m值为0.45 mmol/L.

关键词: 石墨烯, 磷脂, 纳米复合物, 辣根过氧化物酶, 直接电化学

A novel lipid based carbonaceous nanocomposite, 1-palmitoyl-2-oleoyl-sn-glycero-3-phospho-(1'-rac-glycerol) (sodium salt) (POPG) modified graphene (GP) (POPG-GP), was designed and synthesized by a non-covalent method. The nanocomposite was endowed with excellent properties of the two independent components, such as the biocompatibility of POPG and the outstanding electric properties of graphene. Fourier transform infrared (FT-IR) spectra, ultraviolet-visible (UV-vis) absorption spectra, transmission electron microscopy (TEM) were utilized to characterize the structure, morphology and surface property of the as synthesized POPG-GP. It has been found that the modification of POPG on GP could not only assist the dispersion of graphene in aqueous solution, but also endow it with negatively charged, which was favorable for the further immobilization of model enzyme via self-assembly. Based on the electrostatic interaction, the positively charged horseradish peroxide (HRP) could be immobilized onto the surface of POPG-GP to form HRP/POPG-GP/GC electrode. UV-vis and FT-IR spectroscopies were used to monitor the assembly process and demonstrated that HRP had been immobilized without denaturation. The HRP/POPG-GP/GC electrode could commendably realize the direct electron transfer (DET) between electrode and redox enzyme with good electrochemical performance. Moreover, such modified electrode also showed good electrocatalytic response toward the detection of H₂O₂ with high sensitivity, wide linear range, excellent stability and reproducibility. The linear response range for the HRP/POPG-GP/GC was 3.5～210 μmol/L (R=0.999). The detection limit and the sensitivity of the HRP/POPG-GP/GC electrode was calculated to be 1.17 μmol/L (S/N=3) and 356.6 mA·cm^-2·M^-1, respectively. The apparent Michaelis-Menten constant K_m was estimated to be 0.45 mmol/L, indicating a high affinity of HRP to H₂O₂ on POPG-GP. The experiment results demonstrated that POPG-GP not only provided a biocompatible microenvironment for the immobilized HRP, but also supplied a necessary pathway for its direct electron transfer. Therefore, such biocompatible nanocomposite had potential applications in the field of biosensors.

Key words: graphene, phospholipid, nanocomposite, horseradish peroxide, direct electrochemistry

引用此文

张谦, 吴抒遥, 张玲, 茆卉, 刘大亮, 刘洋, 曾向群, 宋溪明, 李景虹. 磷脂修饰化的石墨烯纳米复合物的制备及其直接电化学研究[J]. 化学学报, 2014, 72(3): 388-394.

Zhang Qian, Wu Shuyao, Zhang Ling, Mao Hui, Liu Daliang, Liu Yang, Zeng Xiangqun, Song Ximing, Li Jinghong. Biocompatible Phospholipid Modified Graphene Nanocomposite for Direct Electrochemistry of Redox Enzyme[J]. Acta Chimica Sinica, 2014, 72(3): 388-394.

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磷脂修饰化的石墨烯纳米复合物的制备及其直接电化学研究

Biocompatible Phospholipid Modified Graphene Nanocomposite for Direct Electrochemistry of Redox Enzyme

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