Abstract
A novel electrogenerated chemiluminescence (ECL) immunoassay based on enzyme amplification and magnetic nanoparticle enrichment was developed, and carbohydrate antigen 125 (CA125) was chosen as the analyte. Fe3O4 magnetic nanoparticles loaded with anti-CA125 were synthesized. The sandwich-type immunoassay was performed on the magnetic force-controlled carbon paste electrode via the immunoreactions among glucose oxidase-labeled anti-CA125, CA125, and anti-CA125 on the surface of magnetic nanoparticles. ECL was generated by the reaction between luminol and hydrogen peroxide. Hydrogen peroxide was produced during the enzymatic reaction with glucose and markedly increased in the presence of CA125 antigen. The CA125 concentrations were determined within the range of 0–10 mU mL−1, and the detection limit was 8.0 μU mL−1. The CA125 immunosensor was more sensitive than those previously reported. The proposed ECL method also provided a simple selectivity immunoassay protocol, which was applied in the determination of CA125 in clinical serum samples.
Similar content being viewed by others
References
Mornet S, Vasseur S, Grasset F, Duguet E (2004) Magnetic nanoparticle design for medical diagnosis and therapy. J Mater Chem 14:2161–2175
Corchero JL, Villaverde A (2009) Biomedical applications of distally controlled magnetic nanoparticles. Trends Biotechnol 27:468–476
Li JP, Wei XP, Yuan YH (2009) Synthesis of magnetic nanoparticles composed by Prussian blue and glucose oxidase for preparing highly sensitive and selective glucose biosensor. Sens Actuators B: Chem 139:400–406
Wei H, Wang EK (2008) Fe3O4 magnetic nanoparticles as peroxidase mimetics and their applications in H2O2 and glucose detection. Anal Chem 80:2250–2254
Stamopoulos D (2008) Magnetic nanoparticles utilized in hemodialysis for the treatment of hyperhomocysteinemia: the new challenge of nanobiotechnology. Curr Nanosci 4:302–307
Zirogiannis PN, Stamopoulos D, Bouziotis P, Benaki D, Kotsovassilis C (2008) Utilization of nanobiotechnology in haemodialysis: mock-dialysis experiments on homocysteine. Nephrol Dial Transpl 23:3234–3239
Tsai HY, Hsu CF, Chiu IW, Bor Fuh C (2007) Detection of C-reactive protein based on immunoassay using antibody-conjugated magnetic nanoparticles. Anal Chem 79:8416–8419
Chen HT, Ebnerc AD, Ritterc JA, Kaminskid MD, Rosengarte AJ (2008) Theoretical analysis of a magnetic separator device for ex-vivo blood detoxification. Technology 43:996–1020
Yung CW, Fiering J, Mueller AJ, Ingber DE (2009) Micromagnetic–microfluidic blood cleansing device. Lab Chip 9:1171–1177
Tiefenauer LX, Kossek S, Padeste C, Thiébaud P (1997) Towards amperometric immunosensor devices. Biosens Bioelectron 12:213–223
Tang DP, Yuan R, Chai YQ (2007) Magnetic control of an electrochemical microfluidic device with an arrayed immunosensor for simultaneous multiple immunoassays. Clin Chem 53:1323–1329
Tsourkas A, Hofstetter O, Hofstetter H, Weissleder R, Josephson L (2004) Magnetic relaxation switch immunosensors detect enantiomeric impurities. Angew Chem 116:2449–2453
Tang DP, Yuan R, Chai YQ (2006) Magnetic core–shell Fe3O4@Ag nanoparticles coated carbon paste interface for studies of carcinoembryonic antigen in clinical immunoassay. J Phys Chem B 110:11640–11646
Li JP, Gao HL, Chen ZQ, Wei XP, Yang CF (2010) An electrochemical immunosensor for carcinoembryonic antigen enhanced by self-assembled nanogold coatings on magnetic particles. Anal Chim Acta 665:98–104
Liu ZM, Yang HF, Li YF, Liu YL, Shen GL, Yu RQ (2006) Core–shell magnetic nanoparticles applied for immobilization of antibody on carbon paste electrode and amperometric immunosensing. Sens Actuators B: Chem 113:956–962
Pan J, Yang QW (2007) Antibody-functionalized magnetic nanoparticles for the detection of carcinoembryonic antigen using a flow-injection electrochemical device. Anal Bioanal Chem 388:279–286
Zhang QY, Chen H, Lin Z, Lin JM (2011) Chemiluminescence enzyme immunoassay based on magnetic nanoparticles for detection of hepatocellular carcinoma marker glypican-3. J Pharm Anal 1:166–174
Wang LY, Yang ZH, Zhang Y, Wang L (2009) Bifunctional nanoparticles with magnetization and luminescence. J Phy Chem C 113:3955–3959
Zamfir LG, Geana I, Bourigua S, Rotariu L, Bala C, Errachid A, Jaffrezic-Renault N (2011) Highly sensitive label-free immunosensor for ochratoxin A based on functionalized magnetic nanoparticles and EIS/SPR detection. Sens Actuators B: Chem 159:178–184
Marquette CA, Blum LJ (2008) Electro-chemiluminescent biosensing. Anal Bioanal Chem 390:155–168
Jie GF, Zhang JJ, Wang DC, Cheng C, Chen HY, Zhu JJ (2008) Electrochemiluminescence immunosensor based on CdSe nanocomposites. Anal Chem 80:4033–4039
Zhang ZF, Cui H, Lai CZ, Liu LJ (2005) Gold nanoparticle-catalyzed luminol chemiluminescence and its analytical applications. Anal Chem 77:3324–3329
Lin ZY, Chen JH, Chen GN (2008) An ECL biosensor for glucose based on carbon-nanotube/Nafion film modified glass carbon electrode. Electrochim Acta 53:2396–2401
Dong YP, Cui H, Xu Y (2007) Comparative studies on electrogenerated chemiluminescence of luminol on gold nanoparticle modified electrodes. Langmuir 23:523–529
Jie GF, Wang L, Zhang SS (2011) Magnetic electrochemiluminescent Fe3O4/CdSe–CdS nanoparticle/polyelectrolyte nanocomposite for highly efficient immunosensing of a cancer biomarker. Chem Eur J 17:641–648
Xiong ZG, Li JP, Tang L, Chen ZQ (2010) A novel electrochemiluminescence biosensor based on glucose oxidase immobilized on magnetic nanoparticles. Chin J Anal Chem 38:800–804
Ding CF, Ge Y, Zhang SS (2010) Electrochemical and electrochemiluminescence determination of cancer cells based on aptamers and magnetic beads. Chem Eur J 16:10707–10714
Dietel M, Arps H, Klapdor R, Muller-Hagen S, Sieck M, Hoffmann L (1986) Antigen detection by the monoclonal antibodies CA 19-9 and CA 125 in normal and tumor tissue and patients’ sera. J Cancer Res Clin Oncol 111:257–265
Yan GF, Ju HX, Liang ZC, Zhang TQ (1999) Technical and clinical comparison of two fully automated methods for the immunoassay of CA 125 in serum. J Immun Meth 255:1–8
Reinsberg J, Schultes B, Wagner U, Krebs D (1993) Monitoring cancer antigen 125 in serum of ovarian cancer patients after administration of 131I-Labeled F(ab′)2 fragments of OC125 antibody. Clin Chem 39:891–896
Zeillemaker AM, Verbrugh HA, Hoynck van Papendrecht AAGM, Leguit P (1994) CA 125 secretion by peritoneal mesothelial cells. J Clin Pathol 47:263–265
Yang ZJ, Xie ZY, Liu H, Yan F, Ju HX (2008) Streptavidin-functionalized three-dimensional ordered nanoporous silica film for highly efficient chemiluminescent immunosensing. Adv Funct Mater 18:3991–3998
Kremeskotter J, Wilson R, Schiffrin DJ, Luff BJ, Wilkinson JS (1995) Detection of glucose via electrochemiluminescence in a thin-layer cell with a planar optical waveguide. Meas Sci Technol 6:1325–1328
Dong YP (2010) Electrogenerated chemiluminescence of luminol at a carbon nanotube perfluorosulfonate polymer (Nafion) modified gold electrode. J Lumin 130:1539–1549
Goto Y, Fink AL (1989) Conformational states in β-lactamase: molten-globule states at acidic and alkaline pH with high salt. Biochemistry 28:945–952
Tang DP, Su BL, Tang J, Ren JJ, Chen GN (2010) Nanoparticle-based sandwich electrochemical immunoassay for carbohydrate antigen 125 with signal enhancement using enzyme-coated nanometer-sized enzyme-doped silica beads. Anal Chem 82:1527–1534
Wu LN, Chen J, Du D, Ju HX (2006) Electrochemical immunoassay for CA125 based on cellulose acetate stabilized antigen/colloidal gold nanoparticles membrane. Electrochim Acta 51:1208–1214
Bangar MA, Shirale DJ, Chen W, Myung NV, Mulchandani A (2009) Single conducting polymer nanowire chemiresistive label-free immunosensor for cancer biomarker. Anal Chem 81:2168–2175
Wu LN, Yan F, Ju HX (2007) An amperometric immunosensor for separation-free immunoassay of CA125 based on its covalent immobilization coupled with thionine on carbon nanofiber. J Immunol Methods 322:12–19
Chen SH, Yuan R, Chai YQ, Min LG, Li WJ, Xu Y (2009) Electrochemical sensing platform based on tris(2,2′-bipyridyl)cobalt(III) and multiwall carbon nanotubes–Nafion composite for immunoassay of carcinoma antigen-125. Electrochim Acta 54:7242–7247
Tang DP, Yuan R, Chai YQ (2006) Electrochemical immuno-bioanalysis for carcinoma antigen 125 based on thionine and gold nanoparticles-modified carbon paste interface. Anal Chim Acta 564:158–165
Acknowledgements
The authors gratefully acknowledge the financial support received from the National Nature Science Foundation of China (21165007) and Innovation Project of Guangxi Graduate Education (No. 2011105960703 M22).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Xu, Q., Li, J., Li, S. et al. A highly sensitive electrochemiluminescence immunosensor based on magnetic nanoparticles and its application in CA125 determination. J Solid State Electrochem 16, 2891–2898 (2012). https://doi.org/10.1007/s10008-012-1719-2
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10008-012-1719-2