탄소나노튜브 전자 필름을 이용한 고감도-고선택성 전기화학 글루코스 센서

이승우; 이동욱; 서병관; Seung-Woo Lee; Dongwook Lee; Byeong-Gwuan Seo

Applied Chemistry for Engineering, Vol.33, No.2, 188-194, April, 2022

DOI10.14478/ace.2022.1015 Export Citation

탄소나노튜브 전자 필름을 이용한 고감도-고선택성 전기화학 글루코스 센서

Sensitive and Selective Electrochemical Glucose Biosensor Based on a Carbon Nanotube Electronic Film

이승우^†, 이동욱, 서병관

서울과학기술대학교 정밀화학과

Seung-Woo Lee^†, Dongwook Lee, and Byeong-Gwuan Seo

Department of Fine Chemistry, Seoul National University of Science and Technology, Seoul 01811, Republic of Korea

E-mail:

초록

본 연구에서는 비파괴적 표면 기능기화 통하여 단일벽 탄소나노튜브(SWCNT) 탄소소재의 특성 변화를 최소화 시킬 수 있는 대면적화 공법을 제안하고, 대면적화 된 SWNT 전자 필름 상에 효소를 집적하여 효소와 SWCNT 전자 필름 간 효율적 전자 전달을 연구하였다. p-terphenyl-4,4''-dithiol, dithiothreitol와 SWCNT의 혼합을 통해 SWCNT 전자 필름의 균일도 및 전하 전달 능력을 향상시키고, 분광학적 분석 및 전기화학적 특성을 평가하여 SWCNT 전자 필름의 향상된 전기화학적 특성을 확인하였다. 전자 필름 상에 고분자 전해질 및 포도당 산화환원 효소를 layer-by-layer 기법으로 효율 적으로 집적하여, 최종적으로 음전압 범위에서 구동이 가능한 포도당(glucose) 바이오센서를 구현하였다. 개발된 포도 당 바이오센서는 효소와 SWCNT 전자 필름과의 높은 전하 전달 효율을 바탕으로 -0.45 vs. Ag/AgCl 음전압 범위에서 높은 산화환원 신호를 보였을 뿐 아니라 0~1 mM의 낮은 글루코스 농도 변화에서 약 98 μA/mM⋅cm2의 높은 감도를 보였다. 또한 음전압 구동을 통하여, 산화 반응을 일으킬 수 있는 4종의 방해물질(요산, 아스코르빅산, 도파민, 아세타 아미노펜) 환경에서 4% 이하의 변화를 보여 높은 선택성을 보였다.

This work presents a non-destructive and straightforward approach to assemble a large-scale conductive electronic film made of a pre-treated single-walled carbon nanotube (SWCNT) solution. For effective electron transfer between the immobilized enzyme and SWCNT electronic film, we optimized the pre-treatment step of SWCNT with p-terphenyl-4,4''-dithiol and dithiothreitol. Glucose oxidase (GOx, a model enzyme in this study) was immobilized on the SWCNT electronic film following the positively charged polyelectrolyte layer deposition. The glucose detection was realized through effective electron transfer between the immobilized GOx and SWCNT electronic film at the negative potential value (-0.45 V vs. Ag/AgCl). The SWCNT electronic film-based glucose biosensor exhibited a sensitivity of 98 μA/mM⋅cm2. In addition, the SWCNT electronic film biosensor showed the excellent selectivity (less than 4 % change) against a variety of redox-active interfering substances, such as ascorbic acid, uric acid, dopamine, and acetaminophen, by avoiding co-oxidation of the interfering substances at the negative potential value.

Keywords:Glucose biosensor;Electrochemistry;Carbon nanotube;Glucose oxidase;Electron transfer

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[1] Wang J, Electroanalysis, 13, 983 (2001)

[2] Ronkainen NJ, Halsall HB, Heineman WR, Chem. Soc. Rev., 39, 1747 (2010)

[3] Jang C, Lee HJ, Yook JG, Sensors, 21, 1843 (2021)

[4] Hatada M, Loew N, Inose-Takahashi Y, Okuda-Shimazaki J, Tsugawa W, Mulchandani A, Sode K, Bioelectrochemistry, 121, 185 (2018)

[5] Liu YX, Zhang J, Cheng Y, Jiang SP, ACS Omega, 3, 667 (2018)

[6] Yin ZY, Ji ZW, Zhang WD, Taylor EW, Zeng XP, Wei JJ, ChemistrySelect, 5, 12224 (2020)

[7] Yu YY, Chen ZG, He SJ, Zhang BB, Li XC, Yao MC, Biosens. Bioelectron., 52, 147 (2014)

[8] Liang B, Guo XS, Fang L, Hu YC, Yang G, Zhu Q, Wei JW, Ye XS, Electrochem. Commun., 50, 1 (2015)

[9] Holland JT, Lau C, Brozik S, Atanassov P, Banta S, J. Am. Chem. Soc., 133, 19262 (2011)

[10] Zhang XP, Liu D, Li LB, You TY, Sci. Rep., 5, 9885 (2015)

[11] Yu SY, Myung NV, Front. Chem., 8 (2021)

[12] May P, Laghmari S, Ulbricht M, Membranes, 11, 187 (2021)

[13] Lee D, Ahn HH, Seo BG, Lee SW, J. Sens. Sci. Technol., 30, 229 (2021)

[14] Perez EM, Martin N, Chem. Soc. Rev., 44, 6425 (2015)

[15] Li X, Gao YF, Serpe MJ, Can. J. Chem., 93, 685 (2015)

[16] Park YS, Hembram KPSS, Yoo R, Jang BG, Lee WY, Lee SG, Kim JG, Kim YI, Moon DJ, Lee JK, Lee JK, J. Phys. Chem. C, 123, 14003 (2019)

[17] Niu YZ, He JL, Li YL, Zhao YL, Xia CY, Yuan GL, Zhang L, Zhang YC, Yu C, Microchim. Acta., 183, 2337 (2016)

[18] Wei L, Yushin G, Nano Energy, 1, 552 (2012)

[19] Galban J, Sanz V, Mateos E, Sanz-Vicente I, Delgado-Camon A, de Marcos S, Protein Pept. Lett., 15, 772 (2008)

[20] Devadoss A, Forsyth R, Bigham R, Abbasi H, Ali M, Tehrani Z, Liu YF, Guy OJ, Biosensors, 9, 16 (2019)

[21] Nemiroski A, Christodouleas DC, Hennek JW, Kumar AA, Maxwell EJ, Fernandez-Abedul MT, Whitesides GM, Proc. Natl. Acad. Sci. U. S. A., 111, 11984 (2014)