Skip to main content
Log in

Free-standing electrochemical biosensor for carcinoembryonic antigen detection based on highly stable and flexible conducting polypyrrole nanocomposite

  • Original Paper
  • Published:
Microchimica Acta Aims and scope Submit manuscript

Abstract

A flexible free-standing electrochemical biosensor to detect carcinoembryonic antigen (CEA) is described based on a conducting polypyrrole (PPy) nanocomposite film electrode. The conducting PPy composite was constructed by the sandwiched structure formed by PPy doped with pentaerythritol ethoxylate (PEE) and 2-naphthalene sulfonate (2-NS-PPy) separately via electropolymerization. Gold nanoparticles (AuNPs) were fixed on the PPy composite film by electrodeposition and then connected to CEA aptamer through self-assembly to construct a free-standing electrochemical biosensor breaking away from additional soft substrates and current collector. This PPy composite film-based electrochemical biosensor exhibits satisfying sensing performance for CEA detection, with a linear range from 10−10 g/mL to 10−6 g/mL and a detection limit of 0.033 ng/mL, good specificity and long-term sensing stability (96.8% of the original signal after 15 days). The biosensor also presents acceptable reproducibility with 1.7% relative standard deviation. Moreover, this electrochemical biosensor owns the deformation stability that could bear various deformations (twisting, folding, and knotting) without affecting device’s sensing performance. It can even maintain 99.4% of the original signal under 25% strain deformation. Due to the superior sensing performance, high stability (mechanical deformation and long-term storage), and flexibility, this free-standing electrochemical biosensor proves huge potential in application of flexible and wearable electronics.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Scheme 1
Fig. 1
Fig. 2
Fig. 3
Fig. 4

Similar content being viewed by others

References

  1. Kim J, Campbell AS, de Ávila BE-F, Wang J (2019) Wearable biosensors for healthcare monitoring. Nat Biotechnol 37(4):389–406

    Article  CAS  Google Scholar 

  2. Hong YJ, Jeong H, Cho KW, Lu N, Kim DH (2019) Wearable and implantable devices for cardiovascular healthcare: from monitoring to therapy based on flexible and stretchable electronics. Adv Funct Mater 29(19):1808247

    Article  Google Scholar 

  3. Zhang K, Sun J, Song J, Gao C, Wang Z, Song C, Wu Y, Liu Y (2020) Self-healing Ti3C2 MXene/PDMS supramolecular elastomers based on small biomolecules modification for wearable sensors. ACS Appl Mater Interfaces 12(40):45306–45314

    Article  CAS  Google Scholar 

  4. Nie K, Wang Z, Tang R, Zheng L, Li C, Shen X, Sun Q (2020) Anisotropic, flexible wood hydrogels and wrinkled, electrodeposited film electrodes for highly sensitive, wide-range pressure sensing. ACS Appl Mater Interfaces 12(38):43024–43031

    Article  CAS  Google Scholar 

  5. Kim J, Sempionatto JR, Imani S, Hartel MC, Barfidokht A, Tang GD, Campbell AS, Mercier PP, Wang J (2018) Simultaneous monitoring of sweat and interstitial fluid using a single wearable biosensor platform. Adv Sci 5(10):1800880

    Article  Google Scholar 

  6. Lei Y, Zhao W, Zhang Y, Jiang Q, He JH, Baeumner AJ, Wolfbeis OS, Wang ZL, Salama KN, Alshareef HN (2019) A MXene-based wearable biosensor system for high-performance in vitro perspiration analysis. Small 15(19):1901190

    Article  Google Scholar 

  7. Vargas E, Teymourian H, Tehrani F, Eksin E, Sánchez-Tirado E, Warren P, Erdem A, Dassau E, Wang J (2019) Enzymatic/immunoassay dual-biomarker sensing chip: towards decentralized insulin/glucose detection. Angew Chem Int Ed 58(19):6376–6379

    Article  CAS  Google Scholar 

  8. Jiao L, Yan H, Xu W, Wu Y, Gu W, Li H, Du D, Lin Y, Zhu C (2019) Self-assembly of all-inclusive allochroic nanoparticles for the improved ELISA. Anal Chem 91(13):8461–8465

    Article  CAS  Google Scholar 

  9. Zhang B, Hu X, Jia Y, Li J, Zhao Z (2021) Polyaniline@Au organic-inorganic nanohybrids with thermometer readout for photothermal immunoassay of tumor marker. Microchim Acta 188(3):63

    Article  CAS  Google Scholar 

  10. Achadu OJ, Abe F, Suzuki T, Park EY (2020) Molybdenum trioxide nanocubes aligned on a graphene oxide substrate for the detection of nrovirus by surface-enhanced raman scattering. ACS Appl Mater Interfaces 12(39):43522–43534

    Article  CAS  Google Scholar 

  11. Gholami MD, Sonar P, Ayoko GA, Izake EL (2020) A highly sensitive SERS quenching nanosensor for the determination of tumor necrosis factor alpha in blood. Sens Actuators B: Chem 310:127867

    Article  CAS  Google Scholar 

  12. Hou L, Qin Y, Li J, Qin S, Huang Y, Lin T, Guo L, Ye F, Zhao S (2019) A ratiometric multicolor fluorescence biosensor for visual detection of alkaline phosphatase activity via a smartphone. Biosens Bioelectron 143:111605

    Article  CAS  Google Scholar 

  13. Xu S, Jiang L, Wang J, Gao Y, Luo X (2019) Ratiometric multicolor analysis of intracellular microRNA using a chain hybrid substitution-triggered self-assembly of silver nanocluster-based label-free sensing platform. ACS Appl Mater Interfaces 12(1):373–379

    Article  Google Scholar 

  14. Yu L, Zhang Q, Kang Q, Zhang B, Shen D, Zou G (2020) Near-infrared electrochemiluminescence immunoassay with biocompatible Au nanoclusters as tags. Anal Chem 92(11):7581–7587

    Article  CAS  Google Scholar 

  15. Xu Z, Teng H, Song J, Gao F, Ma L, Xu G, Luo X (2019) A nanocomposite consisting of MnO2 nanoflowers and the conducting polymer PEDOT for highly sensitive amperometric detection of paracetamol. Microchim Acta 186(8):499

    Article  Google Scholar 

  16. Liu N, Song J, Lu Y, Davis JJ, Gao F, Luo X (2019) Electrochemical aptasensor for ultralow fouling cancer cell quantification in complex biological media based on designed branched peptides. Anal Chem 91(13):8334–8340

    Article  CAS  Google Scholar 

  17. Xu Z, Han R, Liu N, Gao F, Luo X (2020) Electrochemical biosensors for the detection of carcinoembryonic antigen with low fouling and high sensitivity based on copolymerized polydopamine and zwitterionic polymer. Sens Actuators B: Chem 319:128253

    Article  CAS  Google Scholar 

  18. Zhou Y, Yin H, Zhao W-W, Ai S (2020) Electrochemical, electrochemiluminescent and photoelectrochemical bioanalysis of epigenetic modifiers: a comprehensive review. Coord Chem Rev 424:213519

    Article  CAS  Google Scholar 

  19. Hui X, Sharifuzzaman M, Sharma S, Xuan X, Zhang S, Ko SG, Yoon SH, Park JY (2020) High-performance flexible electrochemical heavy metal sensor based on layer-by-layer assembly of Ti3C2Tx/MWNTs nanocomposites for noninvasive detection of copper and zinc ions in human biofluids. ACS Appl Mater Interfaces 12(43):48928–48937

    Article  CAS  Google Scholar 

  20. Zhang Y, Lv Q, Chi K, Li Q, Fan H, Cai B, Xiao F, Wang S, Wang Z, Wang L (2021) Hierarchical porous carbon heterojunction flake arrays derived from metal organic frameworks and ionic liquid for H2O2 electrochemical detection in cancer tissue. Nano Res 14(5):1335–1343

    Article  CAS  Google Scholar 

  21. Khoshroo A, Sadrjavadi K, Taran M, Fattahi A (2020) Electrochemical system designed on a copper tape platform as a nonenzymatic glucose sensor. Sens Actuators B: Chem 325:128778

    Article  CAS  Google Scholar 

  22. Xu M, Obodo D, Yadavalli VK (2019) The design, fabrication, and applications of flexible biosensing devices. Biosens Bioelectron 124-125:96–114

    Article  CAS  Google Scholar 

  23. Bariya M, Li L, Ghattamaneni R, Ahn CH, Nyein HYY, Tai L-C, Javey A (2020) Glove-based sensors for multimodal monitoring of natural sweat. Sci Adv 6(35):eabb8308

    Article  CAS  Google Scholar 

  24. Yang Y, Song Y, Bo X, Min J, Pak OS, Zhu L, Wang M, Tu J, Kogan A, Zhang H, Hsiai TK, Li Z, Gao W (2019) A laser-engraved wearable sensor for sensitive detection of uric acid and tyrosine in sweat. Nat Biotechnol 38(2):217–224

    Article  Google Scholar 

  25. Kim W, Lee JS, Jang J (2020) Aptamer-functionalized three-dimensional carbon nanowebs for ultrasensitive and free-standing PDGF biosensor. ACS Appl Mater Interfaces 12(18):20882–20890

    Article  CAS  Google Scholar 

  26. Dağcı K, Alanyalıoğlu M (2016) Preparation of free-standing and flexible graphene/Ag nanoparticles/poly(pyronin Y) hybrid paper electrode for amperometric determination of nitrite. ACS Appl Mater Interfaces 8(4):2713–2722

    Article  Google Scholar 

  27. Gu X, She Z, Ma T, Tian S, Kraatz H-B (2018) Electrochemical detection of carcinoembryonic antigen. Biosens Bioelectron 102:610–616

    Article  CAS  Google Scholar 

  28. Wu Q, Li N, Wang Y, Xu Y, Wu J, Jia G, Ji F, Fang X, Chen F, Cui X (2020) Ultrasensitive and selective determination of carcinoembryonic antigen using multifunctional ultrathin amino-functionalized Ti3C2-MXene nanosheets. Anal Chem 92(4):3354–3360

    Article  CAS  Google Scholar 

  29. Gao F, Zhang N, Fang X, Ma M (2017) Bioinspired design of strong, tough, and highly conductive polyol-polypyrrole composites for flexible electronics. ACS Appl Mater Interfaces 9(7):5692–5698

    Article  CAS  Google Scholar 

  30. Gao F, Song J, Xu Z, Xu L, Guo Y, Miao L, Luo X (2021) All-polymer free-standing electrodes for flexible electrochemical sensors. Sens Actuators B: Chem 334:129675

    Article  CAS  Google Scholar 

  31. Huang K-J, Liu Y-J, Zhang J-Z, Liu Y-M (2015) A sequence-specific DNA electrochemical sensor based on acetylene black incorporated two-dimensional CuS nanosheets and gold nanoparticles. Sens Actuators B: Chem 209:570–578

    Article  CAS  Google Scholar 

  32. Zarei SS, Soleimanian-Zad S, Ensafi AA (2018) An impedimetric aptasensor for shigella dysenteriae using a gold nanoparticle-modified glassy carbon electrode. Microchim Acta 185(12):538

    Article  Google Scholar 

Download references

Funding

This work was supported by Natural Science Foundation of Shandong Province (ZR2019BB008), National Natural Science Foundation of China (21974075), Talent Fund of Shandong Collaborative Innovation Center of Eco-Chemical Engineering (XTCXQN09), the Taishan Scholar Program of Shandong Province of China (ts20110829), and the Science and Technology Benefiting the People Project of Qingdao (20-3-4-53-nsh).

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Fengxian Gao or Xiliang Luo.

Ethics declarations

Conflict of interest

The authors declare no competing interests.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

ESM 1

(DOCX 4446 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Song, J., Teng, H., Xu, Z. et al. Free-standing electrochemical biosensor for carcinoembryonic antigen detection based on highly stable and flexible conducting polypyrrole nanocomposite. Microchim Acta 188, 217 (2021). https://doi.org/10.1007/s00604-021-04859-1

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s00604-021-04859-1

Keywords

Navigation