Skip to main content

Clinical validation of surface-enhanced Raman scattering-based immunoassays in the early diagnosis of rheumatoid arthritis

Analytical and Bioanalytical Chemistry volume 407, pages 8353–8362 (2015)Cite this article

Abstract

We assessed the clinical feasibility of conducting immunoassays based on surface-enhanced Raman scattering (SERS) in the early diagnosis of rheumatoid arthritis (RA). An autoantibody against citrullinated peptide (anti-CCP) was used as a biomarker, magnetic beads conjugated with CCP were used as substrates, and the SERS nanotags were comprised of anti-human IgG-conjugated hollow gold nanospheres (HGNs). We were able to determine the anti-CCP serum levels successfully by observing the distinctive Raman intensities corresponding to the SERS nanotags. At high concentrations of anti-CCP (>25 U/mL), the results obtained from the SERS assay confirmed those obtained via an ELISA-based assay. Nevertheless, quantitation via our SERS-based assay is significantly more accurate at low concentrations (<25 U/mL). In this study, we compared the results of an anti-CCP assay of 74 clinical blood samples obtained from the SERS-based assay to that of a commercial ELISA kit. The results of the anti-CCP-positive group (n = 31, >25 U/mL) revealed a good correlation between the ELISA and SERS-based assays. However, in the anti-CCP-negative group (n = 43, <25 U/mL), the SERS-based assay was shown to be more reproducible. Accordingly, we suggest that SERS-based assays are novel and potentially useful tools in the early diagnosis of RA.

This is a preview of subscription content, access via your institution.

Access options

Buy single article

Instant access to the full article PDF.

USD 39.95

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

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

References

  1. Porter MD, Lipert RJ, Siperko LM, Wang G, Narayana R (2008) Chem Soc Rev 37:1001–1011

    CAS  Article  Google Scholar 

  2. Han XX, Cai LJ, Guo J, Wang CX, Ruan WD, Han WY, Xu WQ, Zhao B, Ozaki Y (2008) Anal Chem 80:3020–3024

    CAS  Article  Google Scholar 

  3. Lee M, Lee S, Lee JH, Lim HW, Seong GH, Lee EK, Chang SI, Oh CH, Choo J (2011) Biosens Bioelectron 26:2135–2141

    CAS  Article  Google Scholar 

  4. Gong JL, Liang Y, Huang Y, Chen JW, Jiang JH, Shen GL, Yu RQ (2007) Biosens Bioelectron 22:1501–1507

    CAS  Article  Google Scholar 

  5. Driskell JD, Kwarta KM, Lipert RJ, Porter MD, Neill JD, Ridpath JF (2005) Anal Chem 77:6147–6154

    CAS  Article  Google Scholar 

  6. Wang G, Park HY, Lipert RJ, Porter MD (2009) Anal Chem 81:9643–9650

    CAS  Article  Google Scholar 

  7. Yang J, Palla M, Bosco FG, Rindzevicius T, Alstrøm TS, Schmidt MS, Boisen A, Ju J, Lin Q (2013) ACS Nano 7:5350–5359

    CAS  Article  Google Scholar 

  8. Li M, Cushing SK, Zhang J, Suri S, Evans R, Petros WP, Gibson LF, Ma D, Liu Y, Wu N (2013) ACS Nano 7:4967–4976

    CAS  Article  Google Scholar 

  9. Li T, Guo L, Wang Z (2008) Biosens Bioelectron 23:1125–1130

    CAS  Article  Google Scholar 

  10. Ni J, Lipert RJ, Dawson GB, Porter MD (1999) Anal Chem 71:4903–4908

    CAS  Article  Google Scholar 

  11. Grubisha DS, Lipert RJ, Park HY, Driskell J, Porter MD (2003) Anal Chem 75:5936–5943

    CAS  Article  Google Scholar 

  12. Lin CC, Yang YM, Chen YF, Yang TS, Chang HC (2008) Biosens Bioelectron 24:178–183

    CAS  Article  Google Scholar 

  13. Xu SP, Ji XH, Xu WQ, Li XL, Wang LY, Bai YB, Zhao B, Ozaki Y (2004) Analyst 129:63–68

    CAS  Article  Google Scholar 

  14. Wang G, Lipert RJ, Jain M, Kaur S, Chakraboty S, Torres MP, Batra SK, Brand RE, Porter MD (2011) Anal Chem 83:2554–2559

    CAS  Article  Google Scholar 

  15. Yoon J, Choi N, Ko J, Kim K, Lee S, Choo J (2013) Biosens Bioelectron 47:62–67

    CAS  Article  Google Scholar 

  16. Chung E, Jeon J, Yu J, Lee C, Choo J (2015) Biosens Bioelectron 64:560–565

    CAS  Article  Google Scholar 

  17. Ko J, Lee C, Choo J (2015) J Hazard Mater 285:11–17

    CAS  Article  Google Scholar 

  18. Gao R, Ko J, Cha K, Jeon JH, Rhie G, Choi J, deMello AJ, Choo J (2015) Biosens Bioelectron 72:230–236

    CAS  Article  Google Scholar 

  19. Ye J, Chen Y, Liu Z (2014) Angew Chem Int Ed 53:10386–10389

    CAS  Article  Google Scholar 

  20. Wang Y, Rauf S, Grewal YS, Spadafora LJ, Shiddiky MJA, Cangelosi GA, Schlucker S, Taru M (2014) Anal Chem 86:9930–9938

  21. Lee S, Chon H, Lee M, Choo J, Shin SY, Lee YH, Rhyu IH, Son SW, Oh CH (2009) Biosens Bioelectron 24:2260–2263

    CAS  Article  Google Scholar 

  22. Huang J, Kim KH, Choi N, Chon H, Lee S, Choo J (2011) Langmuir 27:10228–10233

    CAS  Article  Google Scholar 

  23. Chon H, Lee S, Son SW, Oh CH, Choo J (2009) Anal Chem 81:3029–3034

    CAS  Article  Google Scholar 

  24. Chon H, Lee S, Yoon SY, Chang SI, Lim DW, Choo J (2011) Chem Commun 47:12515–12517

    CAS  Article  Google Scholar 

  25. Chon H, Lee S, Yoon SY, Lee EK, Chang SI, Choo J (2014) Chem Commun 50:1058–1060

    CAS  Article  Google Scholar 

  26. Angenendt P (2005) Drug Discov Today 10:503–511

    CAS  Article  Google Scholar 

  27. Lee M, Kim KH, Park JG, Lee JH, Lim HW, Park MY, Chang SI, Lee EK, Lim DW, Choo J (2012) Biochip J 6:10–16

    CAS  Article  Google Scholar 

  28. Kanda V, Kariuki JK, Harrison DJ, McDermott MT (2004) Anal Chem 76:7257–7262

    CAS  Article  Google Scholar 

  29. Chon H, Lee S, Wang R, Bang SY, Lee HS, Bae SC, Lee H, Kim B, Choo J (2014) RSC Adv 4:32924–32927

    CAS  Article  Google Scholar 

  30. Nijenhuis S, Zendman AJW, Vossenaar ER, Pruijn GJM, van Venrooij WJ (2004) Clin Chim Acta 350:17–34

    CAS  Article  Google Scholar 

  31. Bossuyt X, Coenen D, Fieuws S, Verschueren P, Westhovens R, Blanckaert N (2009) Ann Rheum Dis 68:287–289

    CAS  Article  Google Scholar 

  32. Jaskowski TD, Hill HR, Russo KL, Lakos G, Szekanecz Z, Teodorescu M (2010) J Rheumatol 37:1582–1588

    CAS  Article  Google Scholar 

  33. Chon H, Lee S, Wang R, Bang SY, Lee HS, Bae SC, Hong SH, Yoon YH, Lim D, Choo J (2015) Highly sensitive immunoassay of anti-cyclic citrullinated peptide marker using surface-enhanced Raman scattering detection. Proc SPIE 9523:95230J. doi:10.1117/12.2189760.

  34. Schwartzberg AM, Oshiro TY, Zhang JZ, Huser T, Talley CE (2006) Anal Chem 78:4732–4736

    CAS  Article  Google Scholar 

  35. Wang H, Goodrich GP, Tam F, Oubre C, Nordlander P, Halas NJ (2005) J Phys Chem B 109:11083–11087

    CAS  Article  Google Scholar 

  36. Arnett FC, Edworthy SM, Bloch DA, McShane DJ, Fries JF, Cooper NS, Healey LA, Kaplan SR, Liang MH, Luthra HS (1988) Arthritis Rheum 31:315–324

    CAS  Article  Google Scholar 

  37. Bland JM, Altman DG (1986) Lancet 1:307–310

    CAS  Article  Google Scholar 

  38. Passing H, Bablok W (1983) J Clin Chem Clin Biochem 21:709–720

    CAS  Google Scholar 

Download references

Acknowledgments

This work was supported by the National Research Foundation of Korea (Grant Numbers 2008-0061856 and 2009-00426) and by the Nano Materials Technology Development Program through the National Research Foundation of Korea. The study was funded by the Ministry of Education, Science and Technology (Grant Number 2012M3A7B4035288). H.C. acknowledges the financial support (Grant Number 2013R1A1A2063269) of the National Research Foundation of Korea.

Conflict of interest

The authors declare that they have no competing interests.

Author information

Authors and Affiliations

  1. Department of Bionano Technology, Hanyang University, Ansan, 426-791, South Korea

    Hyangah Chon, Rui Wang, Sangyeop Lee, Dong Woo Lim & Jaebum Choo

  2. Department of Rheumatology, Hanyang University Hospital for Rheumatic Diseases, Seoul, 133-792, South Korea

    So-Young Bang, Hye-Soon Lee & Sang-Cheol Bae

  3. EOne Laboratories, Songdo, 406-840, South Korea

    Sung Hyun Hong & Young Ho Yoon

  4. Department of Chemistry and Applied Biosciences, Institute of Chemical and Bioengineering, ETH Zürich, Vladimir Prelog Weg 1, 8093, Zürich, Switzerland

    Andrew J. deMello

Authors
  1. Hyangah Chon
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Rui Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Sangyeop Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. So-Young Bang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Hye-Soon Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Sang-Cheol Bae
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Sung Hyun Hong
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Young Ho Yoon
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Dong Woo Lim
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Andrew J. deMello
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Jaebum Choo
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Jaebum Choo.

Additional information

Published in the topical collection Raman4Clinics with guest editors Jürgen Popp and Christoph Krafft.

Electronic supplementary material

Below is the link to the electronic supplementary material.

ESM 1

(PDF 1.52 mb)

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Chon, H., Wang, R., Lee, S. et al. Clinical validation of surface-enhanced Raman scattering-based immunoassays in the early diagnosis of rheumatoid arthritis. Anal Bioanal Chem 407, 8353–8362 (2015). https://doi.org/10.1007/s00216-015-9020-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s00216-015-9020-8

Keywords

  • Surface-enhanced Raman scattering
  • Anti-CCP
  • Rheumatoid arthritis
  • Immunoassay
  • Early diagnosis