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

doi:10.7503/cjcu20180283

Abstract

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

CLC Number:

O657.15

TrendMD:

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^†[J]. Chem. J. Chinese Universities, 2018, 39(11): 2386.

Figures/Tables 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

References 44

[1]	Poppi D. A., Moore S. S., Glencross B. D., Aquaculture, 2017, 471, 213—222
[2]	Zee T., Bose N., Zee J., Jennifer N. B., Yang S., Parihar J., Yang M., Damodar S., Hall D., Monique N. O, Ramanathan A., Roy R. G., David W.K., Chi T., Tischfield J., Sahota A., Kahn A., Marshall L. S., Kapahi P., Nat. Med., 2017, 23(3), 288—290
[3]	Treggiari D., Zoccatelli G., Chignola R., Molesini B., Minuz P., Pandolfini T., Food Chem., 2017, 221, 1346—1353
[4]	Zong E. Y., Xiong X., Yang H. S., Li J. Z., Huang P. F., Yin Y. L., Life Sci. Res., 2016, 20(5), 466—470
	(宗恩艳, 熊霞, 杨焕胜, 李建中, 黄鹏飞, 印遇龙. 生命科学研究, 2016, 20(5), 466—470)
[5]	Sercan P. C., Andrew J., Artaches A. K., Brett P., Arianne S., Harald R., Michelle C., Gary R. D., Andrew R. S., Microchem. J., 2015, 121, 141—149
[6]	Thera J. C., Kidd K. A., Dodge-Lynch M. E., Bertolo R. F., Anal. Biochem., 2017, 539, 158—161
[7]	Taniguchi M., Konya Y., Nakano Y., Fukusaki E., J. Biosci. Bioeng., 2017, 124(4), 414—418
[8]	Nakano Y., Konya Y., Taniguchi M., Fukusaki E., J. Biosci. Bioeng., 2017, 123(1), 134—138
[9]	Culea M., Scrob S., Suvar S., Podea P., Has L., Anal. Lett., 2015, 48(1), 37—46
[10]	Omar M. M. A., Elbashir A. A., Schmitz O. J., Food Chem., 2017, 214, 300—307
[11]	Nehmé R., Atieh C., Fayad S., Claude B., Chartier A., Tannoury M., Elleuch F., Abdelkafi S., Pichon C., Morin P., J. Sep. Sci., 2017, 40, 558—566
[12]	Turkia H., Sirén H., Penttilä M., Pitkänen J. P., Talanta, 2015, 131, 366—371
[13]	He J. L., Wu P., Zhu S. L., Li T., Li P. P., Xiang J. N., Cao Z., Talanta, 2015, 132, 809—813
[14]	Xiao H., He J. L., Xiao H., Yang C., Feng Z. M., Yin Y. L., Cao Z., Chinese J. Anal. Chem., 2017, 45(10), 1517—1522
	(肖慧, 何婧琳, 肖昊, 杨婵, 冯泽猛, 印遇龙, 曹忠. 分析化学, 2017, 45(10), 1517—1522)
[15]	Xia S. J, Shao H., Chen G., Chinese J. Food Hygiene, 2008, 20(4), 304—308
	(夏苏捷, 邵泓, 陈钢. 中国食品卫生杂志, 2008, 20(4), 304—308)
[16]	Zhang L., Lu B., Lu C., Lin J. M., J. Sep. Sci., 2014, 37(1/2), 30—36
[17]	Alwael H., Connolly D., Barron L., Paull B.,J. Chromatogr. A., 2010, 1217(24), 3863—3870
[18]	Salimi A., Roushani M., Electroanalysis, 2006, 18(21), 2129—2136
[19]	Zor E., Bingol H., Ramanaviciene A., Ramanavicience A., Eraoz M., Analyst, 2015, 140(1), 313—321
[20]	Wei Z., Yang Y., Xiao X., Zhang W., Wang J., Sens. Actuators B, 2018, 255, 895—906
[21]	Gutierrez F. A., Rubianes M. D., Rivas G. A., J. Electroanal. Chem., 2016, 765, 16—21
[22]	Garcia V. N., Saurina J., Hernandez C. S., Fresenius J. Anal. Chem., 2001, 371(7), 1001—1008
[23]	Stefan V., Staden R. I., Holo L., Sens. Actuators B, 2007, 120(2), 399—402
[24]	Shahrokhian S., Anal. Chem., 2001, 73(24), 5972—5978
[25]	Deore B., Chen Z., Nagaoka T., Anal. Chem., 2000, 72(17), 3989—3994
[26]	Tong S. L, Rechnitz G. A., Anal. Lett., 1976, 9(1), 1—11
[27]	Sugawara A., Matsui D., Yamada M., Asano Y., Lsobe K., J. Biosci. Bioeng., 2015, 119(3), 369—374
[28]	Chauhan N., Narang J., Pundir C. S., Asano Y., Lsobe K., Enzym. Microb. Tech., 2013, 52(4/5), 265—271
[29]	Yin L. T, Lin Y. T, Leu Y. C, Hu C. Y., Sens. Actuators B, 2010, 148(1), 207—213
[30]	Lue C. E, Wang I. S, Huang C. H, Shiao Y. T, Wang H. C, Yang C. M, Hsu S. H, Chang C. Y, Wang W., Lai C. S., Microelectron. Reliab., 2012, 52(8), 1651—1654
[31]	Das A., Ko D. H., Chen C. H., Chang L. B., Lai C. S., Chu F. C., Chow L., Lin R. M., Sens. Actuators B, 2014, 205, 199—205
[32]	Zhang W. M., Feng Y., Diao K. S., Sun L., Hong F., Su Z. X., Hu Y. P., Chem. J. Chinese Universities, 2013, 34(9), 2233—2238
	(张卫民, 冯宇, 刁开盛, 孙丽, 洪芳, 苏智兴, 胡玉平. 高等学校化学学报, 2013, 34(9), 2233—2238)
[33]	Tarasov A., Gray D. W., Tsai M. Y., Shields N., Montrose A., Creedon N., Lovero P., Riondan A. O., Mooney M. H., Biosens. Bioelectron., 2016, 79, 669—678
[34]	Liu D. P., Chu Y. L., Wu X. H., Huang J., Sci. China Mater., 2017, 60(10), 977—984
[35]	Zang Y. P., Di C. A., Zhu D. B., Scientia Sinica Chemica, 2016, 46(10), 1023—1038
	(臧亚萍, 狄重安, 朱道本. 中国科学: 化学, 2016, 46(10), 1023—1038)
[36]	Luo X. L., Xu J. J., Chen H. Y., Chinese J. Anal. Chem., 2004, 32(10), 1395—1400
	(罗细亮, 徐静娟, 陈洪渊. 分析化学, 2004, 32(10), 1395—1400)
[37]	Cao Z., Xiao Z. L., Zhang L., Luo D. M., Kamahori M., Shimoda M., Mater. Sci. Eng. C, 2013, 33(3), 1481—1490
[38]	Iskierko Z., Sosnowska M., Sharma P. S., Benincori T., Souza F. D., Kaminska L., Fronc K., Npworyto K., Biosens. Bioelectron., 2015, 74, 526—533
[39]	Purwidyantri A., Lai H. C., Tsai S. H., Luo J. D., Chiou C. C., Tian Y. C., Cheng C. H., Lin Y. T., Lai C. S., Sens. Actuators B, 2015, 217, 92—99
[40]	Wustoni S., Hideshima S., Kuroiwa S., Nakanishi T., Mori Y., Osaka T., Sens. Actuators B, 2016, 230, 374—379
[41]	Nuzzo R. G., Allara D. L., J. Am. Chem. Soc., 1983, 105(13), 4481—4483
[42]	Nuzzo R. G., Zegarski B. R., Dubois L. H., J. Am. Chem. Soc., 1987, 109(3), 733—740
[43]	Biebuyck H. A., Whitesides G. M., Langmuir, 1993, 9, 1766—1770
[44]	Palmer D. W., Peters T. Jr., Clin. Chem., 1969, 15(9), 891—901