传感器类型
电化学生物传感器
检测对象
过氧化氢(H2O2,PBS缓冲液)、葡萄糖(glucose,PBS缓冲液及人血清)
检测原理
该体系以GCE为换能器,AgNP/F-SiO2/GO修饰层提供催化与电子转导界面。检测H2O2时,H2O2在AgNPs表面发生电催化还原,在−0.3 V产生还原电流,电流随H2O2浓度升高而增大。检测葡萄糖时,GOD作为识别元件选择性催化葡萄糖在O2存在下氧化为葡萄糖内酯并生成H2O2;生成的H2O2再被AgNPs催化还原,形成与葡萄糖浓度相关的安培/CV信号。SiO2包覆GO既隔离GO又稳定AgNPs,AgNPs提供无酶催化放大,使葡萄糖检测通过H2O2间接完成。
检测灵敏度
H2O2: LOD: 4 × 10−6 M (S/N=3);线性范围: 1 × 10−4 M–0.26 M;rY = 0.998。葡萄糖: LOD: 310 μm;线性范围: 2–12 mM;R = 0.996;人血清加标: R = 0.993。
效应效果
H2O2传感器对1×10−3 M H2O2连续10次测量RSD为4.3%,5天后信号仅损失7.1%;在−0.3 V低电位检测可降低其他电活性物质干扰。与电沉积AgNPs/GCE和水热PQ11-AgNPs/GCE相比,峰电位分别正移240 mV和80 mV;与简单电还原Ag+ GCE及PVA-AgNPs/Pt电极相比,峰电流分别增强66.6%和38.8%。葡萄糖传感器对8 mM葡萄糖5次测量RSD为4.1%,优于PtNPs葡萄糖传感器的5.2%;人血清中加标线性R=0.993,6.5 mM时RSD为4.5%。4 ℃保存5天后响应降至初始83%。作者认为该复合电极可用于人血清葡萄糖检测。
传感器的构成
- 基底/换能器电极:玻璃碳电极(GCE),经1.0和0.3 μm氧化铝抛光,作为工作电极与电子转导基底
- 纳米片基底:氧化石墨烯(GO)纳米片,提供大比表面积支撑层
- 包覆层:二氧化硅(SiO2)层,通过溶胶-凝胶法包覆GO,隔离GO并固定后续AgNPs
- 功能化层:3-氨基丙基三乙氧基硅烷(APTES)引入NH2基团,用于吸附或原位还原AgNPs
- 催化/信号层:银纳米粒子(AgNPs),催化H2O2还原并增强电流响应
- 识别元件:葡萄糖氧化酶(GOD),用于葡萄糖传感器中催化葡萄糖氧化生成H2O2
- 固定/成膜材料:壳聚糖(chitosan)和Nafion(0.2%),用于固定GOD/AgNP-A/F-SiO2/GO复合层并稳定电极表面
中文摘要
本文报道了首次在不预先功能化氧化石墨烯(GO)的情况下,通过超声与溶胶-凝胶法结合制备结构明确的二氧化硅包覆GO纳米片(SiO2/GO)。随后用3-氨基丙基三乙氧基硅烷(APTES)对SiO2/GO表面进行氨基(NH2)功能化,得到功能化SiO2/GO(F-SiO2/GO),并作为负载银纳米粒子(AgNPs)的载体,通过两条路线合成AgNP/F-SiO2/GO纳米片:一是直接吸附预制的带负电AgNPs,二是在原位化学还原银盐。透射电镜(TEM)和扫描电镜(SEM)表征了纳米复合物的形貌。结果表明,所得AgNP/F-SiO2/GO对H2O2还原具有显著催化性能。基于该复合物的H2O2传感器具有小于2 s的快速安培响应时间,线性范围为1×10−4 M至0.26 M(rY=0.998),信噪比为3时检出限为4×10−6 M。作者还将葡萄糖氧化酶(GOD)固定于AgNP/F-SiO2/GO修饰的玻璃碳电极(GCE)上构建葡萄糖生物传感器,并证明其可用于人血清中葡萄糖检测。
英文摘要
In this paper, we report on the first preparation of well-defined SiO(2)-coated graphene oxide (GO) nanosheets (SiO(2)/GO) without prior GO functionalization by combining sonication with sol-gel technique. The functional SiO(2)/GO nanocomposites (F-SiO(2)/GO) obtained by surface functionalization with NH(2) group were subsequently employed as a support for loading Ag nanoparticles (AgNPs) to synthesize AgNP-decorated F-SiO(2)/GO nanosheets (AgNP/F-SiO(2)/GO) by two different routes: (1) direct adsorption of preformed, negatively charged AgNPs; (2) in situ chemical reduction of silver salts. The morphologies of these nanocomposites were characterized by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). It is found that the resultant AgNP/F-SiO(2)/GO exhibits remarkable catalytic performance for H(2)O(2) reduction. This H(2)O(2) sensor has a fast amperometric response time of less than 2s. The linear range is estimated to be from 1×10(-4) M to 0.26 M (r=0.998) and the detection limit is estimated to be 4 × 10(-6) M at a signal-to-noise ratio of 3, respectively. We also fabricated a glucose biosensor by immobilizing glucose oxidase (GOD) into AgNP/F-SiO(2)/GO nanocomposite-modified glassy carbon electrode (GCE) for glucose detection. Our study demonstrates that the resultant glucose biosensor can be used for the glucose detection in human blood serum.