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Citation: LIN Yu-Lin, LI Xiao-Juan, ZHANG Xin-Ying, CAO Jie, ZHANG Jian-Hua, CHEN Xiao-Ying. Ru(bpy)₃²⁺/MWCNTs-Nafion-Silica Nanoparticles Modified Electrochemiluminescent Sensor Based on Molecular Imprinting Technique for Detection of 17β-Estradiol[J]. Chinese Journal of Analytical Chemistry, ;2016, 44(10): 1547-1554. doi: 10.11895/j.issn.0253-3820.160395 shu

Ru(bpy)₃²⁺/MWCNTs-Nafion-Silica Nanoparticles Modified Electrochemiluminescent Sensor Based on Molecular Imprinting Technique for Detection of 17β-Estradiol

1.
College of Environmental and Resource, Fuzhou University, Fuzhou 350116, China;
2.
AQSIQ Key Laboratory of Drug Detection, Fujian Entry-Exit Inspection and Quarantine Bureau of P.R.C., Fuzhou 350001, China;
3.
College of Life Sciences, Fujian Agriculture and Forestry University, Fuzhou 350002, China;
4.
Fujian Radiation Environmental Supervision Station, Fuzhou 350013, China

Received Date: 26 May 2016
Revised Date: 8 July 2016

Figures(8)

Environmental endocrine disruptors such as 17β-estradiol, are widely distributed with low concentration in the water, which has great harm to ecosystems and human health. To improve the detection sensitivity of 17β-estradiol, a Ru(bpy)₃²⁺/MWCNTs-Nafion-SiO₂ modified electrode was firstly made by electrostatic adsorption of multi-walled carbon nanotubes (MWCNTs) and ion exchange of Nafion, binding nano-silica and immobilizing Ru(bpy)₃²⁺ on the surface of gold electrode. And then a molecular imprinting-electrochemiluminescence sensor (ECL-MIPs) was acquired by modifying the molecular imprinted membrane with sol-gel method for improving the specific selectivity. Under the optimum conditions (in 0.1 mol/L PBS, pH 7.4) at a scan rate of 100 mV/s and accumulation time of 20 min), there was a good linear relationship between the ECL intensity difference and 17β-estradiol concentration in the range of 0.03-2 μg/L, with a detection limit of 0.006 μg/L. The ECL-MIPs sensor was successfully applied to the determination of 17β-estradiol in the water samples with recoveries from 88.7% to 105.0%.
- Molecular Imprinting,
- Electrochemiluminescence,
- Nano-silica,
- 17β-Estradiol
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Address：Zhongguancun North First Street 2,100190 Beijing, PR China Tel: +86-010-82449177-888

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Figure 1. (A) Cyclic voltammetry curves of bare electrode (a),Multi-walled carbon nanotubes (MWCNTs)-Nafion-SiO₂ modified electrode (b) and MWCNTs-Nafion modified electrodes (c) in 5 mmol/L K₃Fe(CN)₆ and K₄Fe(CN)₆ (containing 0.1 mol/L KCl) solution; (B) Electrochemiluminescence(ECL) behavior of Ru(bpy)₃²⁺/MWCNTs-Nafion-SiO₂ modified electrode (a),Ru(bpy)₃²⁺/MWCNTs-Nafion modified electrode (b) in 0.1 mol/L PBS solution (pH=7.4). Scan rate: 100 mV/s

Figure 2. SEM images of (A) carboxylated MWCNTs,(B) Nafion-SiO₂ and (C) composites (MWCNTs-Nafion-SiO₂)

Figure 3. AFM images of the MIPs,NIPs (A,B are NIPs,respectively; C,D are MIPs before and after eluting respectively)

Figure 4. (A) Cyclic voltammograms of ECL-MIPs sensor before (curve a) and after adsorption of 17β-estradiol (E₂) (curve b). scan rate: 100 mV/s. (B) ECL responses of ECL-MIPs sensor with (curve a) and without (curve b) adsorption of E₂; ECL-NIPs sensor with (curve c) and without (curve d) adsorption of E₂. Concentrations of E₂: 100 μg/L. Butter system: 0.1 mol/L PBS

Figure 5. In 5 mmol/L K₃Fe(CN)₆ and K₄Fe(CN)₆ (containing 0.1 mol/L KCl) solution,Complex impedance polt of (a) bare gold electrode; (b) Ru(bpy)₃²⁺/MWCNTs-Nafion-SiO₂ modified electrode; ECL-MIPs senor before (c) and after (d) template removal; and (e) ECL-MIPs sensor absorbed 100 μg/L E₂. Frequency range: 1~10⁶ Hz

Figure 6. (A) Cyclic voltammogram of different scanning speed (a-g: 20,50,100,200,300,400,500 mV/s,respectively) of ECL electrode ; (B) Effects of different volume ratio of template molecule (100 mg/L E₂) and functional monomer (PTMOS) on ECL intensity of ECL-MIPs sensor in 100 μg/L E₂ solution; (C) Effects of different accumulation time (5,10,15,20,25,30 min) on ECL intensity of ECL-MIPs sensor in 100 μg/L E₂solution; (D) Effects of different pH (5.7,6.2,7.0,7.4,8.0,8.8,9.9) on ECL intensity in 0.1 mol/L PBS solution containing 100 μg/L E₂

Figure 7. (A) The ECL responses of ECL-MIPs sensor to (a) bisphenol A(BPA),(b) estrone (E₁),(c) nonylphenol (NP) and (d) E₂,the inset shows ECL responses of sensor to (a) BPA,(b) E₁ and (c) NP; (B) Reproducibility and stability of ECL-MIPs sensor in 50 μg/L E₂solution

Figure 8. ECL intensity of the sensor with different concentrations of E₂: 0,0.03,0.05,0.1,0.2,0.3,0.6,0.8,1.0,1.2,1.5,1.8 and 2 μg/L (curve a-m),respectively in 0.1 mol/L PBS (pH 7.4) at a scan rate of 100 mV/s,the inset shows the calibration curve for E₂

Ru(bpy)32+/MWCNTs-Nafion-Silica Nanoparticles Modified Electrochemiluminescent Sensor Based on Molecular Imprinting Technique for Detection of 17β-Estradiol

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通讯作者: 陈斌, bchen63@163.com

Ru(bpy)₃²⁺/MWCNTs-Nafion-Silica Nanoparticles Modified Electrochemiluminescent Sensor Based on Molecular Imprinting Technique for Detection of 17β-Estradiol