genomics, proteomics, metabolomics ELISA Enzyme-Linked ImmunoSorbent Assay ECL Electrochemi-luminescence SPR Surface Plasmon Resonance ECL

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21 3 5 1) HPLC GC/MS LC/MS/MS 2), 3) genomics, proteomics, metabolomics 1. PK/TK 2. 3. ELISA Enzyme-Linked ImmunoSorbent Assay ECL Electrochemi-luminescence SPR Surface Plasmon Resonance ECL ECLSulfo-Tag ELISA ECLELISA ECL Fig. 1 Table 1 ECL PK 212

1. Buffer %Serum Table 1 Comparative results of ECL and ELISA assay ECL ELISA Abs 1. Sensitivity&range (mu/ml in human serum) 2.74~6 5 ~ 4.1 1 1 EPO Conc. (mu/ml) (a) ELISA Matrix effect (human serum/buffer ratio at LLOQ) Time (h) Sample expenditure (μl) 2.74/2.74 = 1 4 ~ 5 25 5/12.5 = 4 6 ~ 7 Fig. 1 ECL Signal Buffer %Serum.1 1 1 EPO Conc. (mu/ml) (b) ECL Calibration curve of EPO using ELISA (a) and ECL (b) PK/PD REOPRO Remicade 4) 9) ELISAECLSPR Table 2 EMA 1) FDA 11) White paper 12) Table 2 Comparison of immunogenicity assay ECL ELISA SPR Biacore Characteristics Applied plate assay Popular plate assay Real-time flow-based detection High sensitive Established method Label-free Pros Wide range High sensitive Can detect Low-affinity Abs (early immune response) Can detect Low-affinity Abs Inexpensive equipment Characterize detected Abs High throughput High throughput Not yet established High background Not yet established Cons May not detect all low-affinity Abs? Limited in ability to detect low-affinity Abs Moderate Sensitivity Expensive equipment Low throughput relatively Sensitivity (detection of low-affinity Abs) 57 ± 37 ng/ml 26 ± 92 ng/ml 39 ng/ml 212

EMA 1) ECLSPR ECLSPR ECL HCP, Host Cell ProteinHCP SPRG-CSF Host Cell HCP Host Cell Protein 13) HCP PMDA HCP HCP HCP FcProteinA/GHCP Sulfo-Tag ProteinA/G Fig. 2HCP ECL 39 2. 1 5 ng/mlfda 11) 25 5 ng/ml Fig. 3 Fig. 2 Anti HCP antibody HCP-Biotin Streptavidin Streptavidin coated plate for ECL SULFO-TAG labeled Protein A/G Assay principle of detection of anti-hcp antibodies ECL Signal Fig. 3 1e6 1 1 Ab Conc.(ng/mL) Calibration curve of anti HCP antibodies in 1% human serum SPR SPR 1 G-CSF.3925 µg/ml.6 4.1 SPR QC 112 117QC 117 IgMIgAIgE IgG 212

Response ( = baseline) QC IgMIgAIgE QC IgG 93.5 RU QC 129 RU Fig. 4 QC IgG QCIgG RU 13 12 1 9 8 7 6 5 4 3 2 Fig. 4 QC sample blank sample QC sample Serum sample Anti-IgM Anti-IgA Anti-IgE 3.4 RU 4.6 RU 13.2 RU 225 RU blank sample 118 RU 3.4 RU 6.5 RU 13.7 RU 93.5 RU Sensorgrams of isotyping Anti-IgG 129 RU 2 5 8 1 14 17 2 s Time ( = baseline) FCM DNA T Jurkat cell V V FCM Fig. 5 PI-A 1 3 1 4 1 5 Q1 Q2 Live cells Q3 Q4 1 2 mrna SNPs PCR ECL LC-MS/MS FCM GC- MS 14) 17) FCM PI-A Fig. 5 1 5 1 4 1 3 1 2 1 2 1 3 1 4 1 5 Annexin V FITC-A Live cells (a) Control cells. Q1 Q3 Late apoptotic cells Early apoptotic cells 1 2 1 3 1 4 1 5 Annexin V FITC-A (b) Vinblastine treated cells. Apoptosis detection by flow cytometry of (a) control and (b) vinblastine treated cells Q2 Q4 212

1),, Nature FOCUS, Nature 211 6 3, http://www.natureasia.com/japan/ nature/ad-focus/1163.php 2) Biomarkers and Surrogate Endpoints: Clinical Research and Applications, G. J. Downing ( ), Elsevier (2) 3) FDA critical path initiative report. 4) S. Porter, J. Pharm. Sci., 9, 1 (21). 5) P. Chamberlain and A.R Mire-Sluis, Dev Biol Basel, 112, 3 (23). 6) A. S. Rosenberg, Dev Biol. Basel, 112, 15 (23). 7) H. Schellekens and N. Casadevall, Dev Biol. Basel, 112, 23 (23). 8) H. Frost, Toxicology, 29, 155 (25). 9) A. Kromminga and H. Schellekens, Ann. N. Y. Acad. Sci., 15, 257 (25). 1) European medicines Agency, Guideline on Immunogenicity Assessment of Biotechnology-Derived Therapeutic Proteins, 13 Dec 27, http://www. emea.europa.eu/docs/en_gb/document_library/ Scientific_guideline/29/9/WC53946.pdf 11) Food and Drug Administration, draft Guidance for Industry: Assay Development for Immunogenicity Testing of Therapeutic Proteins, December 29, http://www.fda.gov/downloads/drugs/guidance ComplianceRegulatoryInformation/Guidances/UCM 19275.pdf 12) E. Koren, H. W. Smith, E. Shores, G. Shankar, D. Finco-Kent, B. Rup, Y. C. Barrett, V. Devanarayan, B. Gorovits, S. Gupta, T. Parish, V. Quarmby, M. Moxness, S. J. Swanson, G. Taniguchi, L. A. Zuckerman, C. C. Stebbins and A. Mire-Sluis, J. Immunol. Methods, 333, 1 (28). 13) E. Koren, L. A. Zuckerman and A. R Mire-Sluis, Curr. Pharm. Biotechnol., 3, 349 (22). 14) Food and Drug Administration, Guidance for Industry: Bioanalytical Method Validation, May 21, http://www.fda.gov/downloads/drugs/ GuidanceComplianceRegulatoryInformation/ Guidances/ucm717.pdf 15) European Medicines Agency, Guideline on bioanalytical method validation, 21Jul 211, http://www. ema.europa.eu/docs/en_gb/document_library/ Scientific_guideline/211/8/WC519686.pdf 16) J. W. Lee, V. Devanarayan, Y. C. Barrett, R. Weiner, J. Allinson, S. Fountain, S. Keller, I. Weinryb, M. Green, L. Duan, J. A. Rogers, R. Millham, P. J. O Brien, J. Sailstad, M. Khan, C. Ray and J. A. Wagner, Pharm. Res., 23, 312 (26). 17), 12 1, 23 1 2,, http:// www.pmda.go.jp/ich/e/e16_11_1_2.pdf URL http://www.scas.co.jp/ 541-43 4-6-17 TEL 6-622-181 113-33 3-22-5 TEL 3-5689-1217 212