基于聚二硫二丙烷磺酸膜修饰FET延长栅极的L-胱氨酸传感器

doi:10.7503/cjcu20180283

高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (11): 2386.doi: 10.7503/cjcu20180283

基于聚二硫二丙烷磺酸膜修饰FET延长栅极的L-胱氨酸传感器

杨佳, 张煜杨, 刘陈, 李佳欣, 肖忠良(), 李丹, 张玲, 曹忠()

长沙理工大学化学与生物工程学院, 电力与交通材料保护湖南省重点实验室,微纳生物传感与食品安全检测协同创新中心, 长沙 410114

收稿日期:2018-04-11 出版日期:2018-11-10 发布日期:2018-10-16
作者简介:联系人简介: 曹忠, 男, 博士, 教授, 主要从事纳米生物传感、环境与食品安全检测及装置方面的研究. E-mail: zhongcao2004@163.com; 肖忠良, 男, 博士, 教授, 主要从事环境检测与传感器件及装置方面的研究. E-mail: xiaozhongliang@163.com
基金资助:
国家自然科学基金(批准号: 31527803, 21545010)资助.

L-Cystine Sensor Based on Modification of Extended Gate of FET with Polydithiodipropanesulfonic Acid Membrane^†

YANG Jia, ZHANG Yuyang, LIU Chen, LI Jiaxin, XIAO Zhongliang^*(), LI Dan, ZHANG Ling, CAO Zhong^*()

Collaborative Innovation Center of Micro/nano Biosensing and Food Safety Inspection, Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, China

Received:2018-04-11 Online:2018-11-10 Published:2018-10-16
Contact: XIAO Zhongliang,CAO Zhong E-mail:xiaozhongliang@163.com;zhongcao2004@163.com
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.31527803, 21545010).

摘要/Abstract

摘要：

将场效应晶体管(FET)的栅极金电极(GGE)延长一定距离, 在GGE表面自组装上聚二硫二丙烷磺酸(SPS)膜, 构建了一种可检测L-胱氨酸(L-cystine)的新型传感装置. 该传感界面的SEM表征、电化学性能测试和XPS分析结果表明, 在溶液中带负电荷的SPS聚阴离子膜可通过静电作用吸附结合带正电荷的目标物L-胱氨酸, 形成双电层结构而产生识别一价有机铵离子的膜电位. 该电极在磷酸盐缓冲溶液(pH=5.0)中对L-胱氨酸有良好的电位响应性能, 线性范围为5.0×10^-6~1.0×10^-3 mol/L, 响应灵敏度为(58.25±1.5) mV/-pc(25 ℃), 检出限为2.69×10^-6 mol/L. 该电极响应快(30 s), 重现性及稳定性好. 常见氨基酸如L-甘氨酸、 L-丙氨酸、 L-缬氨酸、 L-天冬氨酸、 L-脯氨酸、 L-苏氨酸、 L-组氨酸、 L-亮氨酸、 L-色氨酸及L-甲硫氨酸等均不干扰电极对L-胱氨酸的测定. 该电极可用于实际猪血清样品中L-胱氨酸的测定, 回收率为91.2%~107.8%, 说明该方法是一种装置简便, 能准确测定L-胱氨酸的新手段.

关键词: L-胱氨酸, 栅极金电极, 场效应晶体管, 聚二硫二丙烷磺酸, 电位传感器

Abstract:

A novel sensing device capable of detecting L-cystine was constructed by designing the gate gold electrode(GGE) of a field effect transistor(FET) to extend a certain distance and self-assembly of polydithiodipropanesulfonic acid(SPS) on the surface of GGE. The topological structure of the modified GGE was characterized by means of scanning electron microscopy. Through electrochemical cyclic voltammetry and impedance analysis together with X-ray photoelectron spectroscopy, the response mechanism of the SPS modified GGE for the L-cystine detection has been well investigated. With electrostatic interaction, the SPS poly-anion membrane with negative charge in aqueous solution could adsorb the L-cystine molecules containing positive charge, which may form a double electric layer resulting in change of membrane potential on the sensing interface by recognition of monovalent organic ammonium ion. The electrode exhibited a nice linear potential performance to L-cystine in the range of 5.0×10^-6~1.0×10^-3 mol/L, with a slope of (58.25±1.5) mV/-pc(25 ℃) and a detection limit of 2.69×10^-6 mol/L. The response time for L-cystine was very fast(30 s). The electrode also had good reproducibility and stability. Almost no interferences from common amino acids such as L-glycine, L-alanine, L-valine, L-aspartate, L-proline, L-threonine, L-histidine, L-leucine, L-tryptophan or L-methionine can be observed. Moreover, the electrode can be applied to the determination of L-cystine in real pig serum samples with recovery rate of 91.2%—107.8%. It shows that the sensing device is expected to become a kind of simple and accurate means for the L-cystine analysis.

Key words: L-Cystine, Gate gold electrode, Field effect transistor, Polydithiodipropanesulfonic acid, Potentiometric sensor

中图分类号:

O657.15

TrendMD:

杨佳, 张煜杨, 刘陈, 李佳欣, 肖忠良, 李丹, 张玲, 曹忠. 基于聚二硫二丙烷磺酸膜修饰FET延长栅极的L-胱氨酸传感器. 高等学校化学学报, 2018, 39(11): 2386.

YANG Jia, ZHANG Yuyang, LIU Chen, LI Jiaxin, XIAO Zhongliang, LI Dan, ZHANG Ling, CAO Zhong. L-Cystine Sensor Based on Modification of Extended Gate of FET with Polydithiodipropanesulfonic Acid Membrane^†. Chem. J. Chinese Universities, 2018, 39(11): 2386.

图/表 14

Fig.1 Schematic diagram for design of extended gate field effect transistor

Fig.2 Schematic diagram of the potentiometric device1. Digital multimeter; 2. regulated power supply; 3. extended gate FET; 4. working electrode; 5. reference electrode; 6. thermostatic controller.

Fig.3 SEM images of electrode surfaces for bare GGE(A), GGE/SPS(B) and GGE/SPS/L-cystine(C)

Fig.4 Schematic illustration of the response process of the electrode

Fig.5 Impedance(A) and cyclic voltammetry(B) plots of the electrodes for bare GGE(a), GGE/SPS(b) and GGE/SPS/L-cystine(c) in the media solution containing 2.0 mmol/L K3[Fe(CN)6]/K4[Fe(CN)6] and 0.2 mol/L Na2SO4

Fig.6 XPS spectra of the electrode surfaces for bare GGE(a), GGE/SPS(b) and GGE/SPS/L-cystine(c)

Table 1 Binding energy(Eb) of different atoms

Electrade	E_b/eV
Electrade	Au	S	O	N	C
GGE	84.27		531.78	401.74	284.80
GGE/SPS	84.38	161.71	532.11	400.09	284.80
GGE/SPS/L-cystine	84.20	161.71	531.65	400.07	284.80

Fig.7 Effect of pH valeus on the sensitivity of GGE/SPS electrode

Fig.8 Schematic diagram of response mechanism for recognition of L-cystine through SPS membrane

Fig.9 Potential response curve and its linear relation plot of GGE/SPS electrode to L-cystine in PBS(pH=5.0)

Table 2 Comparison of performance with different modified electrodes to L-cystine*

Electrode	Method	Linear range/ (μmol·L^-1)	LOD/ (μmol·L^-1)	Selectivity	Reference
Ni-CCE	Amperometry	1.0—450	0.64		[18]
rGO/β-CD/GCE	Amperometry	1.0—100			[19]
GGE/SPS	Potentiometry	5.0—1000	2.69	Good	This work

Fig.10 Dynamic response curve of the electrode to various concentration of L-cystine in PBS(pH=5.0) with the timeConcentration of L-cystine added: A. 0; B. 1.000×10-5 mol/L; C. 5.000×10-5 mol/L; D. 1.000×10-4 mol/L; E. 5.000×10-4 mol/L.

Fig.11 Effect of interfering substance on the GGE/SPS electrodea. L-Cystine; b. L-Gly+L-cystine; c. L-Asp+L-cystine;d. L-Val+L-cystine; e. L-Pro+L-cystine; f. L-Ala+L-cystine;g. L-Thr+L-cystine; h. L-Leu+L-cystine; i. L-Trp+L-cystine;j. L-His+L-cystine; k. L-Cys+L-cystine; l. L-Met+L-cystine.

Table 3 Application of GGE/SPS electrode to determination of L-cystine in pig serum samples(n=3)

Sample	Added/(μmol·L^-1)	Measured/(μmol·L^-1)	RSD(%)	Recovery(%)
1	4.00	4.31	3.68	107.80
2	6.00	6.21	2.27	103.50
3	8.00	8.60	1.73	107.50
4	10.00	9.12	1.63	91.20
5	12.00	11.89	1.40	99.08
6	14.00	14.90	1.21	106.40

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基于聚二硫二丙烷磺酸膜修饰FET延长栅极的L-胱氨酸传感器

L-Cystine Sensor Based on Modification of Extended Gate of FET with Polydithiodipropanesulfonic Acid Membrane^†

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基于聚二硫二丙烷磺酸膜修饰FET延长栅极的L-胱氨酸传感器

L-Cystine Sensor Based on Modification of Extended Gate of FET with Polydithiodipropanesulfonic Acid Membrane†

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L-Cystine Sensor Based on Modification of Extended Gate of FET with Polydithiodipropanesulfonic Acid Membrane^†