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Ultra-low charge transfer resistance carbons by one-pot hydrothermal method for glucose sensing

一步水热法合成超低电荷转移阻抗的碳材料及其葡萄糖检测性能研究

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Abstract

Hydrothermal carbon (HTC) is typically well-dispersed, but it remains a great challenge for HTC to become conductive. Co-doping with heteroatoms has been confirmed to be an effective strategy to significantly promote the electrical conductivity of carbon. Moreover, there is no simple and green method to construct sensitive HTC based electrochemical biosensors until now. In this paper, N and S dual-doped carbon (NS-C) with ultra-low charge transfer resistance is easily synthesized from L-cysteine and glucose in a hydrothermal reaction system. The morphology, structural properties and electrochemical properties of the as-prepared NS-C are analyzed. In comparison with the undoped hydrothermal (UC) modified glassy carbon electrode (GCE), the charge transfer resistance of UC (476 Ω) is ten times the value of NS-C (46 Ω. The developed biosensor shows a better performance to detect glucose in a wide concentration range (50-2500 μmol L-1) with the detection limit of 1.77 ^mol L-1 (S/N=3) and a high sensitivity (0.0554 μA cm-2 μmol-1 L). The apparent Michaelis-Menten constant value of GCE/NS-C/GOx/nafion modified electrode is 0.769 mmol L-1, indicating a high affinity of glucose oxidase to glucose. These results demonstrate that the hydrothermal method is an effective way for preparing high electrical conductivity carbon with excellent performances in biosensor application.

摘要

热碳材料具有较好的水溶性, 但是通常表现为绝缘性, 因此提高水热碳材料的导电性仍然是一个重大挑战. 化学掺杂已经被证实 能够显著提高碳材料的导电性, 但目前尚没有一种简单且绿色的方法制备高灵敏度水热碳基的电化学传感器. 本文在水热反应体系中用 L-半胱氨酸和葡萄糖合成了超低电子转移阻抗的氮硫掺杂碳材料, 随后分析了材料的形貌、结构和电化学性质. 氮硫掺杂碳修饰电极电 子转移阻抗(46 Ω)大约是非掺杂碳修饰电极(476 Ω)的1/10. 氮硫掺杂碳材料制备的葡萄糖传感器具有较宽线性范围(50–2500 μmol L−1), 低的检测限(1.77 μ mol L−1, S/N=3)和高的灵敏度(0.0554 μ A cm−2 μmol −1 L). GCE/NS-C/GOx/nafion电极的米氏常数为0.769 mmol L−1, 表 明N S-C 负载的葡萄糖氧化酶(GOx)对葡萄糖具有较高亲和力. 本研究提出以水热法合成具有高电导性的碳材料, 并应用于高性能的葡萄糖传感器.

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Acknowledgements

This work was supported by the National Basic Research Program of China (973 Program, 2014CB931900), UCAS Young Teacher Research Fund (Y55103NY00, Y55103EY00, and Y25102TN00), Beijing Natural Science Foundation (Z160002), and The Chinese Academy of Sciences Key Project Foundation (KFZD-SW-202).

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Authors and Affiliations

  1. College of Materials Science and Opti-Electronic Technology, University of Chinese Academy of Sciences, Beijing, 101408, China

    Botao Hu  (胡博韬) & Jen-Tsai Liu  (刘仁材)

  2. School of Electronic, Electrical and Communication Engineering, University of Chinese Academy of Sciences, Beijing, 101408, China

    Ching-Jung Chen  (陈靖容) & Zhan Zhao  (赵湛)

  3. State Key Lab of Transducer Technology, Institute of Electronics, Chinese Academy of Sciences, Beijing, 100089, China

    Zhan Zhao  (赵湛)

  4. Department of Electric Engineering, I-Shou University, Kaohsiung, 82445, Taiwan

    Shwu Jen Chang  (张淑真)

  5. Cardiovascular Surgery, Department of Surgery, Kaohsiung Veterans General Hospital, Kaohsiung, 82445, Taiwan

    Pei-Leun Kang  (康沛伦)

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  1. Botao Hu  (胡博韬)
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  6. Pei-Leun Kang  (康沛伦)
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Corresponding authors

Correspondence to Jen-Tsai Liu  (刘仁材) or Ching-Jung Chen  (陈靖容).

Additional information

Botao Hu received his bachelor degree from Anhui Normal University. He is now a master candidate at the University of Chinese Academy of Sciences (UCAS) and his research is focused on the carbon materials.

Jen-Tsai Liu is an associate professor at the University of Chinese Academy of Sciences. He received his bachelor degree in 2002 and master degree in 2004 from I-Shou University, and his PhD in 2010 in chemical and materials engineering from Central University, Taiwan. His current research has been mainly focused on biosensors and bioelectrics.

Ching-Jung Chen is an associate professor at the University of Chinese Academy of Sciences. She received his bachelor degree in 2002 and master degree in 2004 from I-Shou University, and her PhD in 2010 in electrical engineering from Central University, Taiwan. Her current research has been mainly focused on biosensors, bioelectrics and biomaterials.

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Hu, B., Liu, JT., Chen, CJ. et al. Ultra-low charge transfer resistance carbons by one-pot hydrothermal method for glucose sensing. Sci. China Mater. 60, 1234–1244 (2017). https://doi.org/10.1007/s40843-017-9104-9

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