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1 RESEARCH Precise Research. Proven Results. AR226-1745 m a Analytical Report I 3M EnvironmentalTechnology and Safety Services II Analysis of Perfluorooctanesulfonate in Mallard and Quail Egg Yolk Exygen Report No. 023-070 m Testing Laboratory a Exygen Research 3058 Research Drive State College, PA 16801 1 Requester William K. Reagen, Ph.D. 3M Environmental Technology and Safety Services Building 2-3E-09 PO Box 33331 St. Paul, MN 55133-3331 PAGE 1 OF 5 F 814.272.1019 exygen.com 1 lntroduction Results are reported for the analysis of total perfluorooctanesulfolnate (PFOS) in mallard and quail egg yolk samples. Also reported is the PFOS contained in each of the three fractions of egg yolk: very low density lipoprotein (VLDL), phosvitin, and lipovitellin. This study was conducted in accordance with the analytrcalphase protocolgiven in Attachment E. 2 Sample Receipt The samples were submitted in plastic bags, labeled with magic marker and typed print. A copy of all sample log-in information is presented in Attachment A Twelve mallard egg yolk samples and twelve quail egg yolk sample:; were received on 06/01/02. The samples were shipped frozen on dry ice via Federal Express ( FedEx). The twelve mallard yolk samples were combined and homogenized into one sample. The same was done for the twelve quail yolk samples. The samples were stored frozen from lime of receipt until analysis. Four mallard albumen and shell membrane samples and four quail albumen and shell membrane samples were also received on 06/01/02. These sampl'es were not analyzed as part of this study. 3 Methods - Analytical and Preparatory 3.1 Sample Preparation 3.1.1 Total PFOS Content A 1.0 g sample was used for the extraction procedure. Twenty-five milliliters of methanol were - - added to the sample. The sample was placed on a wrist-action shaker for 15 minutes and then centrifuged at 2000 rpm for 10 minutes. A five milliliter aliquot of the sample was taken and 0.5 g of carbon was added. The sample was shaken then allowci!d to sit. Each sample was filtered and analyzed by LC/MS/MS electrospray. 3.1.2 PFOS Content in Yolk Fractions A 5.0 g sample was used for the fractionation. Ten milliliters of ;ii solution containing 0.67 M - MgS04,1 mM phenylmethanesulfonylfluoride (PMSF), and 2 pM leupeptin were added to the sample. The sample was shaken for 2 minutes and then the suspension was transferred to a centrifuge tube. The sample was centrifuged at 200,000 x g at 4C for 24 hours. The sample was then separated into 2 segments: the very low density lipo~irotein(VLDL) and the high density fraction (HDF). The VLDL was dissolved in a solution containing20 mM Tris-HCI, 1!jOmM NaCI, 0.2 mM EDTA, 1 rnM PMSF, and 5 pM leupeptin. The HDF was resuspended in (a solution containing 0.45 M MgS04,1 mM PMSF, and 2 pM leupeptin. Both VLDL and HDF fractions were centrifuged at 200,000 x g at 4C for 16 hours. The VLDL was then dissolved in a solution containing 20 mM Tris-HCI, 150 mM NaCI, 0.2 mM EDTA, 1 mM PMSF, and 5 pM leupeptin and stored at 4C. The HDF was dissolved in a solution containing 0.45 M MgSO,I, 1 mM PMSF, and 2 pM PAGE 2 OF 5 leupeptin and then two volumes of cold water was added dropwise ,and then stored overnight at 4C. The HDF supernatant (lipovitellin) was decanted and diluted with cold water and stored overnight at 4C. The HDF precipitate (phosvitin) was dissolved in a solution containing 0.4 M MgS04, 1 mM PMSF, and 2 pM leupeptin and then diluted with cold water and stored overnight at 4C. The lipovitellin and phosvitin were then recovered by centrifugation at 106,000 x g at 4C for 1 hour and dissolved in a solution containing 1 M NaCI, 5 mM Tris-HCI, 1 mM PMSF, and 2 1M leupeptin. All of the resulting precipitates (-1.0 g) from each fraction were used for the extraction - - procedure. Twenty-five milliliters of methanol were added to the sample. The sample was placed on a wrist-action shaker for 15 minutes and then centrifuged at 2000 rpm for 10 minutes. A five milliliter aliquot of the sample was taken and 0.5 g of carbon was added. The sample was shaken then allowed to sit. Each sample was filtered 'and analyzed by LC/MS/MS electrospray 3.2 Sample Analysis by LC/MS/MS In High Pressure Liquid Chromatography (HPLC), an aliquot of extract is injected and passed through a liquid-phase chromatographic column. Based on the a,ffinity of the analyte for the stationary phase in the column relative to the liquid mobile phase, the analyte is retained for a characteristic amount of time. Following HPLC separation, mass spectrometry provides a rapid and accurate means for analyzing a wide range of organic compoimds. Molecules are ionized, fragmented, and detected. The ions characteristic of the compound is observed and quantitated against standards. Each sample was analyzed in duplicate. An HP1000 system interfacedto a Micromass Quattro Ultima system was used to analyze the sample extracts. A gradient elution through a Jones Chromatography Genesis C-8 50 x 2.1 mm x 4pm column was used for separation. The following gradient was performed: Mobile Phase (A): Mobile Phase (B): iime 0.0 0.4 1 .o 7.0 7.5 9.0 9.5 14.0 2mM Ammonium Acetate in Type I Watcer Methanol - %A - %B 60 40 60 40 10 90 10 90 0 100 0 100 60 40 60 40 The following parameters were used for operation of the mass spectrometer: Parameter Ionization Mode Polarity Transitions Monitored Setting Electrospray Negative 499->99 PAGE3OF5 Gas Temperature Drying Gas (N2) 350C 7.0 Umin 4 Analysis 4.1 Calibration A 6-point calibration curve was analyzed at the beginning, throughout, and at the end of the analytical sequence for PFOS. The calibration points were preparmefdor PFOS at 0.1, 0.2, 0.5, 1.0, 2.0, and 5.0 ng/mL. The instrument response versus the concentration was plotted for each point. Using linear regressionwith l l x weighting, the slope, ,y-interceptand coefficient of determination (P) were determined. A calibration curve is acceptakile if ? 2 0.990. For the results reported here,'calibration criteria were met. The calibration curves are included in the raw data in Attachment C. 4.2 Surrogates Surrogate spikes are not a component of the analytical method. 4.3 Laboratory Control Spikes Laboratory control spikes in the analytical set were prepared by adding a known concentration of the analytes to control egg yolk samples. Laboratory control spikes are used to assess method accuracy. The laboratorycontrol spikes must show remveries between 70-130% or the data is rejected. For the results reported here, the spikes were within the acceptable range. 4.4 Matrix Spikes Matrix spikes were not included with this study. 4.5 Sample Related Comments Duplicate injections were performed for all sample analyses. Please see Attachment B for a detailed listing of the analytical re!t;ults. Results are reported in parts per billion (ng/g) for PFOS. Samples are disposed of one month after the report is issued unless otherwise specified. All electronic data is archived on retrievable media and hard copy reports are stored in data folders maintained by Exygen. Hardcopy data is stored for a minimum of five years. 3M Environmentalwill be notified 30 days prior to the disposal of hardcopydata. PAGE40F5 7 Attachments 7.1 Attachment A: Chain of Custody 7.2 Attachment B:Analytical Results 7.3 Attachment C: Raw Analytical Data 7.4 Attachment D: Study Personnel 7.5 Attachment E: Analytical Phase Protocol a 8 Signatures PAGE 5OF5 r IC I 1 L L I L I 0201613 0201614 (Composite) (Composite) See Original Login See Original Looin Exygen Research Sample Login Report Study Number: Protocol: 023-070 NA EGG YOLK NA EGGYOLK . NA RICK K 6-4-02 RICK K 6-4-02 Page 1 of 1 FREEZER 8 FREEZER 8 See Original Login See Original Login Composite of samples: 201551-201 562 Composite of samples: 201 563-201 574 Verified By/Date: 4-y-uz Printed 6/4/2002 ch I Exygen Research Sample Login Report I I Studv Number: I Protocol: 023-070 NA Page 1 of 3 0201551 E01-1379-31882 6-1-02 21115 EGG YOLK NA 0201552 E01-1379-31883 6-1-02 21:15 EGG YOLK NA 0201553 E01-1379-31884 6-1-02 21:15 EGG YOLK NA 0201554 E01-1379-31885 6-1-02 21:15 EGG YOLK NA 0201555 E01-1379-31895 6-1-02 21115 EGG YOLK NA 0201556 E01-1379-31896 6-1-02 21115 EGG YOLK NA 0201557 E01-1379-31897 6-1-02 21115 EGG YOLK NA 0201558 E01-1379-31898 6-1-02 21:15 EGG YOLK NA 0201559 E01-1379-31939 6-1-02 21115 EGG YOLK NA 0201560 E0l-1379-31943 6-1-02 2135 EGG YOLK NA 0201561 E01-1379-31947 6-1-02 21115 EGG YOLK NA 0201562 E01-1379-31951 6-1-02 21115 EGG YOLK NA . .n.m_n...c.c-?.,._ , --.r r r d .-.- .-,-,a O-.~-C-?-O , f--?.--e-?-?.?. ..-?c , !-=-c-cv.-n-!.% . . .?..!.A. 0201564 E01-1378-31639 6-1-02 21:15 EGG YOLK NA 0201565 E01-1378-31640 6-1-02 21115 EGG YOLK NA 0201566 E01-1378-31641 6-1-02 2135 EGG YOLK NA 0201567 E01-1378-31654 6-1-02 21:15 EGG YOLK NA 0201568 E01-1378-31655 6-1-02 21:15 EGG YOLK NA LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 IAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 !-A.W- -!?..C-*.!C.-C- n- 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 LAWRENCE 0 6-3-02 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 . .C!.?!=C?C!?- p-. . FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A '-DRY !CE-.A. F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. -_ .f!.?rd .in.. c. !.?!=c?!=R.-Q !!-ti! . Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Verified By/Date: d-2-02 Printed 6/3/2002 c I ~ f zt Exygen Research Sample Login Report Study Number: 023-070 - Protocol: NA Page 2 of 3 6-3-02 0201570 E01-1378-31657 6-1-02 21115 EGG YOLK NA LAWRENCE 0 FREEZER 8 6-3-02 0201571 E01-1378-31694 6-1-02 21:15 EGG YOLK NA LAWRENCE 0 FREEZER 8 6-3-02 0201572 E01-1378-31698 6-1-02 21:15 EGG YOLK NA LAWRENCE 0 FREEZER 8 6-3-02 0201573 E01-1378-31702 6-1-02 21:15 EGG YOLK NA LAWRENCE 0 FREEZER 8 6-3-02 0201574 E0l-1378-31706 6-1-02 21115 EGG YOLK NA LAWRENCE 0. ' FREEZER 8 6-3-02 0201575 E01-1379-31940 6-1-02 21~15 EGG ALBUMEN NA LAWRENCE 0 FREEZER 8 6-3-02 I 1 I I I 1 I 0201576 E01-1379-31944 6-1-0221:15 EGGALBUMEN NA LAWRENCE 0 6-3-02 FREEZER 8 0201577 E01-1379-31948 6-1-02 21:15 EGG ALBUMEN NA LAWRENCE 0 6-3-02 FREEZER 8 0201578 E01-1379-31952 6-1-02 21115 EGG ALBUMEN NA LAWRENCE 0 6-3-02 FREEZER 8 0201579 E01-1378-31695 6-1-02 21115 EGG ALBUMEN NA LAWRENCE 0 6-3-02 FREEZER 8 0201580 E01-1378-31699 6-1-02 21115 EGG ALBUMEN NA ---.--. --. .-.- -..-- - !??!??<.8? . . . . !=!??-???!?-???!?? , E-?-!?? ? ? . ? c . ~~ FCC A! P.!!ME*J~ J.! _*.. LAWRENCE 0 _ 6-3-02 ~~~ ~ !-A.W- .!?..F_M.C.-!= r-! FREEZER 8 ! ___ - C. !.?.!=_C?C!?..e ! 6-3-02 0201582 E01-1378-31707 6-1-02 21115 EGG ALBUMEN NA LAWRENCE 0 6-3-02 FREEZER 8 0201583 E01-1379-31942 6-1-02 21:15 EGG SHELL NA LAWRENCE 0 FREEZER 8 MEMBRANE 6-3-02 0201584 E01-1379-31946 6-1-02 21:15 EGG SHELL NA LAWRENCE 0 FREEZER 8 MEMBRANE 6-3-02 0201585 E01-1379-31950 6-1-02 21115 EGG SHELL NA MEMBRANE - LAWRENCE 0 6-3-02 FREEZER 8 0201586 E01-1379-31954 6-1-02 21115 EGG SHELL NA LAWRENCE 0 FREEZER 8 MEMBRANE 6-3-02 -. .- Verified By/Date: 6-3-0~ F-DRY ICE-A F-DRY I C E A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A `-DRY !CE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-in. Stored in FREEZER 8 until 1 Log-In. [Storedin FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. !Sto.e! in FREEZER 8 En!?! ! Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-in. Stored in FREEZER 8 until Log-In. Printed 6/3/2002 m 0201587 0201588 0201589 0201590 E01-1378-31697 E01-1378-31701 E01-1378-31705 E01-1378-31709 6-1-02 21:15 6-1-02 21:15 6-1-02 21115 6-1-02 21:15 Exygen Research Sample Login Report Study Number: 023-070 Protocol: NA EGG SHELL NA LAWRENCE 0 MEMBRANE 6-3-02 EGG SHELL NA LAWRENCE 0 MEMBRANE 6-3-02 EGG SHELL NA LAWRENCE 0 MEMBRANE 6-3-02 EGG SHELL NA LAWRENCE 0 MEMBRANE 6-3-02 FREEZER 8 FREEZER 8 FREEZER 8 FREEZER 8 Page 3 of 3 F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A F-DRY ICE-A Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. Stored in FREEZER 8 until Log-In. - - I_-. I - -I , Printed 6/3/2002 513 1l2002 Project: E01-1379 . 3M ENVIRONMENTAL LABORATORY CONTRACT LABORATORY WORK ORDER BY SAMPLE Contract Lab@): EXYGEN 1 of 2 Requester: Robideau, Rochelle R (0002-03E-09) Completion Date: Department: 502180 Site Source: Project Lead: Rwhelle R. Robideau Project Number: Phone Number: 65 1-778-7065 Date Received: 101412001 Email Address: inobideau@mmm.com a- Project Description:N. Bobwhite Reproduction (Eggs) Ship Date: Comments: / NOTE: MISC SERV = Protein separation to be conducted by Exygen Research. 3M Sample ~ ~~~~ E01-1379-3 1882 Analysis Code MI SC-SERV Sampled Date Sample Description ~ 61 131200 1 10 DDm a.i. 230 H Yolk Analvtical Method . Comoonenls Misc. Services Misc. Services ~~~ ~~ Analvsis Due Date 6130i2002 EO 1-1379-3 1883 Analvsis Code MISC-SERV - EO 1 1379-31884 Analysis Code MI SC-SERV E01-1379-3 1885 Analvsis Code MISC-SERV EO 1-1379-3 1895 Analysis Code MISC-SERV EO 1-1379-31896 Analysis Code MISC-SERV 6/13/200 1 10 DDm a.i. 232 H Yolk Analvtical Method Comoonenls Misc. Services Misc. Services 611 31200 1 10 m m a i . 234 H Yolk Analvtical Method ComDonenB Misc. Services Misc. Services 611 31200 1 10 DDm a.i. 236 H Yolk Analvtical Method Comwnenls Misc. Services Misc. Services ~~ ~ ~ ~~ 611312001 10 DDm a.i. 229 I Yolk Analvtical Method ' Comoonenls Misc. Services Misc. Services 6/13/2001 10 m m a.i. 231 I Yolk Anahtical Method Componenls Misc. Services Misc. Services / AnalvsiiDue Date 613012002 Analvsis Due Date 613012002 / . Analvsis Due Date 6130l2002 Analvsis Due Date 613012002 ./- Analysis Due Date 613 012002 E01-1379-31897 Analysis Code MI SC-SERV E01-1379-31898 Analysis Code MISC-SERV E01- 1379-31939 Analwis Code MISC-SERV 611312001 10 m m a.i. 233 I Yolk Analvtical Method ComDonenB Misc. Services Misc. Services 611312001 10 Dom a.i. 235 I Yolk Anahtical Method Comoonenb Misc. Services Misc. Services 6/21/2001 10 DDm a.i. 226 J Yolk Analvtical Method CornDonenis Misc. Services Misc. Services Analysis Due Date 613 012002 . Analvsis Due Date 613012002 Analvsis Due Date 6l3Ol2002 - 513 1l2002 3M ENVIRONMENTAL LABORATORY CONTRA(JT LABORATORY WORK ORDER BY SAMPLE 2 of2 Project: E01-1379 (cont.) 3M Sample ~ ~~ E01-1379-3 1940 Analvsis Code Sampled Date Sample Description 6/2 112001 10 Dum a.i. 226 J Albumen Analytical Method Corn ponen b MISC-SERV Misc. Services Misc. Services Contract Lab@):EXYGEN ,, Analysis Due Date 6/30/2002 EO 1-1379-31942 Analvsis Code MISC-SERV 6/21/2001 10 uDm a.i. 226 J Shell Membrane Analvtical Method Cornoonen ts Misc. Services Misc. Services Analysis Due Date 613012002 EOI-1379-3 1943 Analvsis Code MISC-SERV 6/2 1/2001 10 Dum a.i. 230 J Yolk Analytical Method Cornponen b Misc. Services Misc. Services Analysis Due Date 613012002 E01-1379-3 1944 Analvsis Code MISC-SERV 612112001 10 uDm a.i.230 J Albumen Analytical Method ' Cornponenb Misc. Services Misc. Services Analysis Due Date 6/30/2002 EO 1- 1379-31946 Analysis Code MISC-SERV 612 11200 1 10 DDm a.i. 230 J Shell Membrane Analvtical Method Corn oonen b Misc. Services Misc. Services Analysis Due Date 613012002 EO 1-1379-31947 Analvsis Code PFOS - EO 1 1379-31948 Analvsis Code PFOS 612 112001 10 Dum ai. 232 J Yolk Analytical Method Corn oonenb PFOS by ESMS PFOS 6/21/2001 10 uum a.i. 232 J Albumen Analytical Method Corn oonen b PFOS by ESMS PFOS Analys,is Due Date 613012002 Analysis Due Date 613 012002 E01-1379-3 1950 Analwis Code PFOS E01- 1379-31951 Analpis Code PFOS E01 -1 379-3 1952 Analvsis Code PFOS E01-1379-31954 Analwis Code PFOS 6/21/2001 10 DDm a.i. 232 J Shell Membrane Analvtical Method Components PFOS by ESMS PFOS 6/21/2001 10 Dum a.i. 234 J Yolk Analvtical Method Cornoonenb PFOS by ESMS PFOS 612 112001 10 Dum a.i. 234 J Albumen Analvtical Method Cornoonen ts PFOS by ESMS PFOS 612 1I200 1 10 DDm a.i. 234 J Shell Membrane Analytical Method Cornoonenb PFOS by ESMS PFOS Analysis Due Date 613012062 Analysis Due Date 613012002 Anal& Due Date 613 012002 Analysis Due Date 6/30/2002 - - 3M Environmental Labor Form 38778 - PWO Shipping Addrear: 3M Bidg 2-3E-09 935 BushAvenue E??? Company Robideau, Rochelle R 3M U City, State, Zip Telephone# , h S , 778 70hS Special Instructions andlor Specific Regulatory Requirements: (method. limit of detection. reporting units, etc.) Item I #I Client Sample Identification I 1. b0 m m a.i. 230 H Yolk 2. 10 ppm a.i. 232 H Yolk 3. 10 ppm a.i. 234 H Yolk 4. 10 ppm a i 236 H Yolk 5. 10 ppm a.i. 229 I Yolk 6. 10 ppm a.i. 231 I Yolk 7. 10 ppm a.i. 233 I Yolk 8. 10 ppm a.i. 235 I Yolk 9. 10 ppm a.i. 226 J Yolk I (10ppm a.i. 226 J Albumen ~__ ~ FAX # 1 Date Available ~ Date Due ]Contract Lab \I w+,G - N7- w- r ----- I&YGd I I I I I I Analysis Reauested: Complete below. Attach any associated information. I 131882 31883 31884 31885 31895 31896 31897 31898 31939 131940 Time d Sampled k/13/01 I I b/13/01 b/13/01 b/l3/Ol 5/13/01 5/13/01 5/13/01 5/13/01 ,5/21/01 b/21/01 I I Matrix/ Media z -0 I- Original~ AccompanyinQSamples Last Page - Originator See Reverse Side for Instructions a Environmental Laboratory ,, Chain of Custody /Request for Laboratory Analytical R 3M Env. Lab Project # I (method. limit of detedion. reporting units.-elc.) I I I Preservatives: I I I I I I I I I I I I Analysis Requested: I Completebelow. Attach any associated Information. Item #, Client Sample Identification 1. ho DDm a.i. 230 J Albumen 2. bo ppm a.i. 230 J Shell Membrane 3. 10 ppm a.i. 232 J Yolk 4. 10 ppm a.i. 232 J Albumen 5. 10 pprn a.i. 232 J Shell Membrane 13. 10 ppm a.i. 234 J Yolk 7. 10 ppm a.i. 234 J Albumen 8. 10 ppm a.i. 234 J Shell Membrane 9. 10. I . __ 3M IlMS# b1944 131946 31947 31948 31950 31951 31952 31954 Date Time Sampled Sampled k/21/01 I I b/21/Ol I I 1/21/01 4/21/01 5/21/01 5/21/01 5/21/01 5/21/01 Matrix/ Media I I - I i Page 3 0 f 2 _ Original- A m p a n y - Samples Last Page - Originator See Reverse Side for l n s t r u d i i o 513 112002 3M ENVIRONMENTAL LABORATORY C O N T R A m LABORATORY WORK ORDER BY SAMPLE 1 of2 Project: E01-1378 Contract Lab(s): EXYGEN Requester: Robideau, Rochelle R (0002-03E-09) Completion Date;: . Department: 502180 Site Source: Project Number: Date Received: 10/4/2001 w' Project Description: Mallard Reporduction (Eggs) I Ship Date: Comments: Project Lead: Rochelle R. Robideau Phone Number: 651-778-7065 Email Address: i:rrobideau@mmm.com . / NOTE: MISC SERV = Protein separation conducted by Exygen Research. 3M Sample E01-1378-31638 Analysis Code MISC-SERV EO 1-1378-3 1639 Analvsis Code MI SC-SERV Sampled Date Sample Description 611 31200 1 10 uurn a.i. 230 H Yolk Analvtical Method . ComDonents Misc. Services Misc. Services 611 31200 1 10 uurn a.i. 232 H Yolk Analvtical Method Componenb Misc. Services Misc. Services ~~ ~ Analvsis Due Date 613012002 / . Analysis Due Date 613 012002 ~~ - EO 1-1378-3 1640 Analvsis Code MISC-SERV EO 1-1378-3 1641 Analwis Code MISC-SERV 6l13l2001 10 uum a.i. 234 H Yolk Analvtical Method Cornmnen b Mise. Services Misc. Services 6l13l200 1 10 Dum a.i. 236 H Yolk Analvtical Method Cornmnenb Misc. Services Misc. Services Analvsis Due Date . 613012,002 Analysis Due Date 613012002 - E01-1378-31654 Analvsis Code MISC-SERV ~ ~~ ~~ EO 1- 1378-31655 Analysis Code MISC-SERV 61 131200 1 10 DDm a.i. 229 I YOk Analvtical Method CornDonen tr Misc. Services Misc. Services ~ ~ ~~ 6113/2001 10 Dum a.i. 231 I Yolk Analvtical Method Components Misc. Services Misc. Services Analvsis Due Date 6f3012902 Analvsis Due Date 613012002 E01-1378-3 1656 Analvsis Code MISC-SERV 61 131200 1 10 Dum a.i. 233 I Yolk Analvtical Method CornDonen ls Misc. Services Misc. Services Analysis Due Date 613 Of20_02 E01-1378-3 1657 Analysis Code MISC-SERV EO 1-1378-31694 Analysis Code MISC-SERV 6113f2001 10 uurn a.i. 235 I Yolk Analvtical Method CornDonen b Misc. Services Misc. Services 6121f2001 10 uum a.i. 230 J Yolk Analvtical Method CornDonen b Misc. Services Misc. Services Analvsis Due Date 6130f2002 Analysis Due Date 6l3012002 513 112002 3MENVIRONMENTAL LABORATORY CONTRACT LABORATORY WORK ORDER BY SAMPLE 2 of2 Project: E01-1378 (cont.) 3M Sample Sampled Date Sample Description EO1-1378-31695 Analysis Code MISC-SERV 6/2112001 10Dum a.i. 230J Albumen Anahtical Method ComDonents Misc. Services Misc. Services Contract Lab@):EXYGEN .,, Analysis Due Date 613012002 - EOI-1378-31697 Analwis Code MISC-SERV 6/2112001 10mrn a.i. 230J Shell Membrane Analytical Method Comaonenb Misc. Services Misc. Services Analysis Due Date 61300QQ2 E0l-1378-31698 Analvsis Code MISC-SERV 612l/2OO1 10Dum a.i. 232J Yolk Analytical Method Components Misc. Services Misc. Services Analysis Due Date 613012002 EO1-1378-31699 Analwis Code MISC-SERV 612 11200 1 10mma.i. 232J Albumen Analytical Method Componen b Misc. Services Misc. Services Anal& Due Date 613012002 EO 1-1378-31701 Analysis Code MISC-SERV 6/2lROO1 10mrn a.i. 232J Shell Membrane Analytical Method Com ponen ls Misc. Services Misc. Services Analysis Due Date 613012002 EO 1-1 378-31702 Analwis Code PFOS 612 11200 1 10o m a.i. 234J Yolk Analvtical Method Componenls PFOS by ESMS PFOS / Analvsis'Due Date 6130l2002 EO 1- 1378-31703 Analvsis Code PFOS E01-1378-31705 Analysis Code PFOS 612 11200 1 10uDm a.i. 234J Albumen Analvtical Method ComDonen b PFOS by ESMS PFOS ~~ ~~ 6121I200 1 10 m m a.i. 234 J Shell Membrane Analytical Method ComDonents PFOS by ESMS PFOS Analysis Due Date 613 012002 / . Analysis Due Date 6130l2002 EO 1- 1378-31706 Analwis Code PFOS E01-1378-31707 Analysis Code PFOS 612 11200 1 10DDm a.i. 236J YOk Analvtical Method Componen b PFOS by ESMS PFOS 6 / 2 112001 10DDm a.i. 236J Albumen Analvtical Method Components PFOS by ESMS PFOS Analysis Due Date 613012002 , . Analysis Due Date 613012002 EO1-1378-31709 Analysis Code PFOS 6/21/2001 10m m a.i. 236 J Shell Membrane Analvtical Method Com aonenls PFOS by ESMS PFOS Analysis Due Date 613012002 . Form 38778 ~ PWO I Project IDlProject Name I Shipping Address: Telephone: 3M Bidg 2-3E-09 Sample Receiving: (651) 778-4948 Template # 335 Bush Avenue St Pau1,MN 55106 Alternate: (651) 778-6751 FAX: (651) 7786176 . 5 IDrnind I b a '",C". L I - Y Dept. # (main) Mailing Addressnnn7 -nqF-ns City, State, Zip cT lTelephone# h51 778 7nhs Soecial instructions andlor Specific Re-gulator-yReq.uirements: (method. limit of detection. reporting units. e1c.l FAX ## I I II I I Anialysis Requested: Temperature: 'C Other Assoclaled CoCs Page I_ O*f 0 Received on Ice Original -AccompanyingSamples Last Page - Originatw See Reverse Side for Instructions 3M Environmental Labor Form 30770 - PWO Shipping Address: 3M Bldg 2-3E-09 935 Bush Avenue St Pau1,MN 55106 Telephone: Sample Receiving:(651) 778-4 ' Analysis Requested: Complete below. Attach any associated Information. , Samole Condition UDon Receipt: Temperature: 'C 0 Acceptable 0 Other: 0 Received on Ice Copier IO Page> 01 Original -AccompanyingSampler Commenls: Last Page - Originalor See ReverseSide for lnslruclions I I ~ II RESEARCH Precise Research. Proven Results. Sample "Condition Upon Receipt" Form Protocol # A/# Exygen Study # 023 - 0 70 Date & Time Received 6-/ d 3 27LN . Condition of Samples /-Pr, 2cr - # 1 Temporary Storage Location rI - P 1 Initials & Date i,/ 4 -/-f?z I May 24, 200213 T: 800.2812219 F: 814.272.1 019 E E c I t 11 L L L L I L IE m I I I Ir, c mi 8 I I Exygen Research Sample Login Report I Protocol: NA I I I I I 6-5-02 I I Page 1 of 1 !Markets #33.State I Printed 6/5/2002 *,-j ; . - .- THANK YOU FOR SHOPPIING P .I WEIS MARKETS 4! 33 STATE COI.LEGE, PA \ a Itcn Price 79 F .79 ~ 1.00 - .. Q .21 i I .I - 7 ...,. ., . , . . . 9 C A N SAVE voir $ $ ' s EVERYDAY . . . $ WEIS CLUB HEHBERS U HAVE THE POWER TO SHUE IORE THIS IS AN EXACT COPY OF THE ORIGINAL DOCUMENT." ,p .) d-5-(:j i DATE--,- .. lm RESEARCH Precise Research. '.. Proven Results. Summary of PFOS Residue Found (ppb) in Combined Mallard Egg Yolk Samples Sponsor Analyte Found Fort Level Recovery ID na (Reagent Control) (ppb) NQ -IlPPb) (%) - na (Reagent Control)" NQ na (Reagent Control) NQ na (Reagent Control)" NQ na (Matrix Control) NQ na (Matrix Control)" na (Matrix Control) na (Matrix Controlp na (LCS) NQ - NQ - NQ 108 100 108 na (LCS) 111 100 111 na (LCS) 103 100 103 na (LCS) ** 100 53600 100 100 **A 52300 - ** Dup 52600 - ** DupA 52500 - NQ = Result is above the detection limit of - 0.5 ppb but below the quantitiition limit of 10 ppb. A Duplicate Injection **composite of samples E01-1378-31638,31639,31640,31641,31654,31655,31656,3165'7,31694,31698,31702,31706 . F 814.231.1580 RESEARCH Precise Research. Proven Results. Summary of PFOS Residue Found (ppb) in Combined Quail Egg Yolk Samples Sponsor ID na (Reagent Control) Analyte Found (ppb) NQ Foirt. Level l(ppb) Recovery (%) - na (Reagent Control)'+ na (Reagent Control) na (Reagent Control)A na (Matrix Control) na (Matrix Control)A na (Matrix Control) na (Matrix Control)A na (LCS) na (LCS) - NQ NQ -- NQ NQ - NQ - NQ - NQ 104 100 104 102 100 102 na (LCS) 106 100 106 na (LCS) ** 109 75000 100 109 **A 74300 ** Dup 48700 ** DupA 49900 - NQ = Result is above the detection limit of - 0.5 ppb but below the quantitation limit of 10 ppb. A Duplicate Injection *+composite of samples E01-1379-31882,31883,31884,31885,31895,31896,31897,318!~~8,31939,31943,31947,31951 F 814.231.1580 In RESEARCH Precise Research. Proven Results. 1 Summary of PFOS Residue Found (ppb) I in Mallard*/Quail** Egg Yolk Fractions - Sponsor Analyte Found Fort. Level Recovery I ID (ppb) (ppb) ("/O) na (Reagent Control) ND na (Reagent Control)A ND na (Reagent Control) ND na (Reagent Control)A ND na (Matrix Control)-VLDL 13.5 na (Matrix Control)-VLDLA 14.3 na (Matrix Control)-Phosvitin NQ na (Matrix Control)-PhosvitinA NQ na (Matrix Control)-Lipovitellin NQ na (Matrix Control)-LipovitellinA NQ *-Mallard VLDL 41 800 *-Mallard VLDLA 42500 *-Mallard Phosvitin 3600 *-Mallard PhosvitinA 3580 *-Mallard Lipovitellin *-Mallard LipovitellinA 891 0 8830 - **-Quail VLDL 39700 - **-Quail VLDLA **-Quail Phosvitin 39900 815 **-Quail PhosvitinA 838 **-Quail Lipovitellin 1300 **-Quail LipovitellinA 1340 - - ND = Result is below the detection limit of 0.5 ppb. - NQ = Result is above the detection limit of 0.5 ppb but below the quantitirtion limit of 10 ppb. A Duplicate Injection + composite of samples E01-1378-31638,31639,31640,31641,31654,31655,31656,31657', 31694,31698,31702,31706 *+composite of samples E01-1379-31882,31883,31884,31885,31895,31896,31897,318SI8,31939,31943,31947,31951 F 814.231.I580 E n 3058 Research Drive State college, PA 16801 RESEARCH T: (814) 272-1039 F: (814) 231-1580 STUDY PERSONNEL LOG I PROTOCOL NA EXYGEN STUDY 023-070 1 PRINTED NAME SIGNATURE 1 INITIALS .1 1 1 II ill June 28,2001/1 ANALYTICAL PHASE PROTOCOL ANALYTICAL PHASE TITLE EXTRACTION OF POTASSIUM PERFLUOROOCTANESULFONATE FROM MALLARD AND QUAE EGG YOLK FOR ANALY5;IS USING HPLC- ELECTROSPRAY/MASS SPECTROMETRY SPONSOR 3M Environmental Technology and Safety Services Building 2-3E-09 PO Box 3333 1 St. Paul, MN 55133-3331 DATA REQUIREMENTS Analy-tical Method Requirements PERFORMING LABORATORY Exygen Research (Exygen) 3058 Research Drive Stiite College, PA 16801 Phone 814-272-1039 Exygen Research Page 1 of 39 Title: EXTRACTION OF POTASSIUM PERFLUOROOCTPiNESULFONATE! FROM MALLARD AND QUAIL EGG YOLK FOR ANALYSIS USING HPLCELECTROSPRAYMASSSPECTROMEiiTRY , TABLE OF CONTENTS Page TABLE OF CONTENTS.......................................................................................................... 2 1. PURPOSE...................................................................................................................... 3 2. REFERENCEMATERIAL ............................................. ........................................... 3 3. SPONSOR................................................. ........................ ...........................................4 4. TESTING FACILITY (PERFORMINGLABORATOItY...................................... 4 5. PROPOSEDEXPERIMENTALTIME-FRAME...................................................... 4 6. SAMPLEPROCESSING, STORAGEAND IDENTIFICATION..........................4 7. ANALYTICALMETHOD......................................................................................... 5 8. EXPERIMENTALDESIGN....................................................................................... 5 9. RECORDS.................................................................................................................... 5 10. DATA AND REPORT ..................................................... ........................................... 6 11. COSTS................................................................................ ........................................... 6 12. PROTOCOL APPROVAL..........................................................................................7 APPENDIX: ANALYTICAL METHODS ................................. ........................................... 8 Exygen Research Page 2 of 39 Title: EXTRACTION OF POTASSIUM PERFLUOROOCTANliWJLFONATE FROM MALLARD AND QUAIL EGG YOLK FOR ANALYSIS USING HPLCELECTROSPRAYMASS SPECTROMlXRY 1. PURPOSE The purpose of this study is to analyze mallard and quail egg yolk samples and their fractions for residues of perfluorooctanesulfonate (PFOS) using methods entitled, "Lipovitellin, Phosvitin, and Very Low Density Lipoprotein (VLDL) Isolation from Chicken and Japanese Quail Egg Yo`lk" and "Determination of Peduorooctanesulfonate in Egg Membrane, Albumen and Yolk by L C M S M S." Both methods can be found in the Appendix. 2. REFERENCE MATERIAL The following analytical standard will be used: Test Material PFOS Lot Number 215 Tl3D Chemical name and structure of the compound is presented below. PFOS Chemical Name: IUPAC Name: CAS Number: Molecular Weight: Perfluorooctanesulfonat e 1-Octanesulfonic acid, 1,1,2,2,3,3,4,4,5,5,6,6,7,7,8,8,8heptadecafluoro-, potassium salt 2795-39-3 499 (C8Fi7S03-) 0 0 m e : The neutral molecule and standard from which the PFOS (anion) is obtained is perfluorooctanesulfonate potassium salt [C817S0&], molecular weight 538. A record of test and reference substance receipt, storage conditions, and a record of use will be maintained at Exygen. Forms documenting chain-of-custody and shipping records for tracking of the test substances will be included as part of the raw data package. Exygen Research Page 3 of 39 All standarddtest substances and any prepared solutions must be identified with a unique label or number on the container or cross-referenced to the container. HAZARD INFORMATION A current MSDS for the chemical(s) used in this study will be maintained at the testing facility. 3. SPONSOR 3M Environmental Technology and Safety Services Building 2-3E-09 PO Box 33331 St. Paul, MN 55133-3331 Sponsor Representative: Bill Reagen 4. TESTING FACILITY / PERFORMING LABORA'rORY Exygen Research 3058 Research Drive State College, PA 16801 Project Manager: Emily R. Decker, Exygen 5. PROPOSED EXPERIMENTAL TIME-FRAME Analytical Start Date Analytical Termination Date Report Issued June 3, 2002 June 21,2002 July 3 1, 2002 6. SAMPLE PROCESSING, STORAGE AND IDENTIFICATION All mallard egg yolk samples received will be combined into one composite sample using a blender. The same process will also be used for all of the quail egg yolk samples. Each sample will be assigned a unique sample identification number at Exygen, which will be used for tracking and identification of the samples. The samples will be stored in a tempemme-monitored freezer, maintained at < -10" C, except. when removed for extraction and analysis as described in the method. The: samples will be kept isolated fiom the test substance di.iring storage. Sample receipt and storage location and conditions during the study will be: documented. All samples and any resulting sample extracts will be identified. with a unique label or sample number. Such identification will be either on the: container or cross-referenced to the container. Exygen Research Page 4 of 39 7. ANALYTICAL METHOD The composite mallardquail egg yolk samples will be ctxtracted and analyzed first according to the analytical method titled "Determination of Periluorooctanesulfonate in Egg Membrane, Albumen and Yolk by LCMSMS" to determine the total amount of PFOS in each sample. Then the mallardquail composite yolk samples will be separated into three liactions using the method "Lipovitellin, Phosvitin, and Very Low Density Lipoprotein (VLDL) Isolation from Chicken and Japanese Quail Egg Yolk." Each fraction will then be extracted and analyzed according to the method "Determination of Peffluorooctanesulfonate in Egg Membrane, Albumen imd Yolk by LCMSMS". 8. EXPERIMENTAL DESIGN Samples obtained by 3M Environmental will be shipped to Exygen Research for analysis. Samples will be extracted and analyzed at Exygen according to method, "Determination of Perfluorooctanesulfonate in Egg Membrane, Albumen and Yolk by LCMSMS." ` Methods to control bias will include assay of untreated control samples, fortification of untreated control samples to obtain rc;.:coverydata, and replicate analysis of fortifed samples to provide an indication of reproducibility. Fortification will be made to the matrix prior to extract ion. The average recovery and relative standard deviation of the fortified samples will be calculated. If necessary, apply a standard test for outliers. If an outlier exists, then it may be excluded from the statistical analysis. Also, the average residue found and standard deviation for each matrix will be cailculated. 9. RECORDS Records to be maintained include, but are not liimited the following (as appropriate) : 1. Sample tracking sheet(s) 2. Sample receipt records, storage history, and chains of custody 3 . History and preparation of standards (stock, fortification, calibration) 4. Description of any modifications to the method 5. Instrument run sheets, bench-sheets or logs 6. Analytical data tables 7. All chromatographic and instrumental conditions 8. Sample extraction and analysis dates 9. A complete listing of study personnel, signatures and initials 10. Chronological presentation of all study correspond'ence 11. Any other data necessary for the reconstruction of the study All chromatograms will contain the following: a. Sample identification, date, arrow or other indication of the area of interest, and injection number corresponding to the run. Exygen Research Page 5 of 39 I 1 b. Additionally, fortifications will include the fortification level of the analyte. c. Analytical standard chromatograms will additionally include the concentration (e.g., pg/ml, ng/mL, ppb, ppt, etc.). Each data set will contain information on tempera.tures, flow rates, column parameters, gases, instrument parameters, and instrument type, etc. 10. DATA AND REPORT 1. All raw data and the original signed protocol will be maintained in the study file. This data includes the laboratory notebooks, imalytical standard solution preparation, sample chain of custody sheets, sample work sheets, chromatograms, calibration curves, and any other alppropriate data generated. 2. A report will be issued by Exygen at the completicrn of the study according to the Sponsor's specifications. The report contents should include, but not limited to: 1. Objectives and procedures stated in the protoco I 2. Analytical and statistical methods used 3. Reference materials identified by name, lot, purity, and other characteristics 4.Name of performing laboratory and analytical start and termination dates 5. Tables containing all applicable data 6. All chromatographic and instrumental conditioris 7. A complete listing of Exygen study personnel 11. COSTS The total cost for performance of the study will be $30,000.00. Exygen Research Page 6 of 39 12. PROTOCOL APPROVAL II Project Manager, Exygen Sponsor, 3M /&gzif/& Bill Reagen m Exygen Research Page 7 of 39 APPENDIX: ANALYTICAL MFTEIODS A, "Determination of Perfluorooctanesulfonatein Egg Membrane, Albumen and Yolk by LC/MS/MS" B. "Lipovitellin, Phosvitin, and Very Low Density Lipoprotein (VLDL) Isolation from Chicken and Japanese Quail Egg Yolk" * Exygen Research Page 8 of 39 .. -.. . . .. . ,. -. . . .I . 8 I - TITLE Determination of Perflu rooctanesulfonatein Egg Membrane. ..;lbumenand Yolk by I I AUTHORS Emily Stauffer and John Flaherty II .. I d * . D A IS~SUED Janhary 2,2001 SPONSOR 3M Environmental Laboratory Building 2-3E-09 PO Box 33331 St. Paul, MN 55133-3331 . .. PERFORMING LABORATORY , . .. . Centre Analytical Laboratories, Inc. (Centre:) 3048 Research Drive State College, PA 16801 -C1"NTRESTUDY NUMBER 023-015 .. . CENTRE METHOD NUMBER . OOM-023-015 f. _TOTAL NUMBER OF PAGES .. 28 .. .- .. i Exygen Research Page 9 of 39 Centre Method No: 00M-023-015 s II MANAGEMENTAPPROVAL HI I 1: As per 4d CER 792.3,method development is not required to be conducted in compliance i with Good Laboratory Practices. However, the wo$ Was in conformancewith applicable r. standard operating procedures and general GLP regulations. r I I1 3)blOI 111 Date Principal Investigator. Centre Analytical Laboratories,,h c . /5ohnFlaherty 1 Laboratory Manager . Date Centre Analytical Laboratories, Inc. ! .- 4-rttCtjl-O( 1111 Date - Centre Analytical Laboratories, Inc. Ill insor Represhtative . ?!MEnvbnmental Laboratory . .. . Exygen Research t Page 2 I Page 10 of 39 IIII ' 'IU -1 I II . . . . . . . -. . Centre Method No: OOh-023-015 TABLE OF CONTENTS . I I i ! . 1. SUMMARY................... ........*........................................................ 6 2. EXPERIMENTAL'COMPOUNDS.........+. ............................... :...............7 3. CHEMICALS AND SUIF'PLLES ..................I..... ......".........;..............7 3.1. CmhuCALs ................................................................................................................................................ 7 3.2. ~ANDARD.9........................................................................................... 1.................................... .;.............7 33. EQUIPMENT SuppuEs.............................................................. :......................................................... 8 3.4. SOLUTION.S....;....................................................................................................................................8....... 35. PREPARATIOONFST~(:K. FORTIFICATIONA.NDCuremnQNSOLUTION...S..................................... ;.....9 3.5.1. Stock Solutwn......................................... .............................. ......................................................... 9 3.5.2. FortificationSolutions............................................... ....-..............................................................9.. 3.5.3. &libration Stanthirds..................................................................................................................... 9 4. METHOD............ ............................................................. ............... 10 . . 4.1. 4.2. FSALMOPWLDEPIRAOGCRE.A.S..M.S..I..N.......G.......................................................................................................... .................................................................... ..................................................................... 1010 4.3. SAMPLE-mON, ............................................................................................................................. 10 4.3.1 Egg Membrane......................................... .................................... ..................................................11 4.3.2. Egg Yo& md.4a-n .................................................................................................................. 11 4.4. 4 . ANALYSrS 4.1.. L ~ BYWLcSs/yMstse/mMsan..d....O...p..e..r..a..t.i.n...g...C...o...n..d...i.t.i.o...n..s...(.T...u...r.b...o..l.o...n..r..p...r.t..i.y..).....................................................:......................,...............1122 1 I 4.4:2. Example TuneFile Parameters ............................. ....................................... :........... 13 4.4.3. CalibmtionProcedures.......................................................;......................................................... I3 4.4.4. Sample Analysk................................................................................................................................ 14 45. pERIT)RMMa a m ........................................................................................................................ 15 I 4.6. TIMEREQUIRED ANALYSIS................................................................................................... :...........16 5. .CALCULATIONS............................... I........-...".................................!.......16 6; SAFETY............... ..........................................i....-..................................... 17 TABLES........................................................................................................................ 18 F'IGURES..................... -................................;..-..........................'.. 22 .. Centre Analytical Laboratories: Inc. Study +Y 023-015 Page 3 Exygen Research Page 11 of39 . Illll I Ill .. . I I Centre Method No: 00M-023-015 .... . = LIST OF T U L E S 6 TABLE? suMMARy OF RIscovERlEs FAR PFos cpmEGG . MEMBRANE................................ .....i.......................................................... 19 !Ic. f,' TABLE II: . MSUEMMBMRAARNYEO..F....R...E....C...O...V....E...R...I...ES FO:..R....P...F...O...S....I.N.....M....A...L...L...A...R...D.....E...G...G........ 19 I i: I . TABLEq:SUMMAR.YOF RECOVERIES FOR PFOS IN QUAILEGG YOLK..r................ :........................................................................... 20 TABLE IV:SuMMA,R.YOF RECOVERIES FOR PFos IN MALLAN) EGG 1I111 . YOLK ............:................. ............................................................................ 20 llll .. 1l1'11 TABLE V S w Y OF R I X O a R E S FOR PFOS IN QUAIL EGG , I . . ALBUMEN...................................................................................................... 2.1 . 1, 2 . ' TABLEv1:SUMMARY OF RIXOVERIES FOR PFOS INMALLARD EGG I AWBUMEN............................... ..................................................................... 21 I llll 111 111 I I ... - '. .. '.I c I : . '< .. I 1 .. ,.' I 'I .- .- Centre Analytical Labontories, Inc. Study # 023-015 I . I. . ' Page4 i Exygen Research I i ', I I .. ,. . .. j .- ii . j ,- t - .. *. c Centre Method No: OOM-023-015 LIST OF FIGURES I I Figure 1: Representative Chromatogramof a Quail Egg Membrane Control................23 * Figure 2: RepresentativeChromatogramof a Maliard Egg hkmbrane Control............23 ! Figure 3: RepresentativeChrornatogramofa Quail Egg Yolk Control......................... 24 Figure 4 Representative Chrotnatogramofa MallardEgg yolk Control........... 24 Figure 5: RepresentativeChromatogramof a Quail Egg Albumen Control..................25 Figure 6: Rep-ksentativeChrornatogramofa Mallard Egg Albumen Control ..............25 Figure 7: R10epnrgelsgen(ptap.tbiv).e...C...h...r.o..r..n..a..t.o...g..r.a..m....o...f..a....Q...u..a..i.l..E...g..g....M....e..m...b...r.a..n..e...C...o...n..t.r..o..i..F...o..rtified at 26 Figure 8: Representative Chrornatogkm of a Mallard Egg Membrane Control Fortified at . 10.0nglg (ppb)................................................................. ............ .......26 - Figure 9: Representative Chrornato,k of a Quail Egg Yolk Control Fortified at . 1O.D nglg.(p.pb)............. ............................ i.................................................... '27 Figure.10: Representative Chromatogram of a Mallard Egg Yolk Control Fortified at . . 10.0 ngg (ppb)....................... ..................... .................................................. 27 c . ;. . . Figure.11: Representative Chromatogram ofa Quail Egg Albumen Control Fortified at ,. .. . 10.0nglg (ppb).............................. :............................................................... 28 ! ?i . 1 . .' Egufe 12: Representative Chromatogram of a Mallard Egg Albumen Control.Fortifiedat h I- 10.0 nglg (ppb) .............................................................................................. 28 I t .. .. !. .: . . .. Page 5 Exygen Research Page 13 of 39 - t ! I 111 111 'rn I I 1 1 I I I I. Ill II i 1 I I. i 1 t ; .. C&h Method No: OOM-023-015 i I . 1. SUMMARY . - 1 .This document details perfluorooctanesulfonate a method (PFOS) in of egg analysis for rhe residual determination of membrane, albumen and yolk. The chemical formula of the analyte is given in Section 2 of this method. i, 1I Perfluorooctanesulfonatc is exbracted from each matrix with methanol (MeOH). For egg membrane samples, the methanol extract is Passed through a membrane filter. For egg albumen and yolk samples, a 0.5g of carbon is added to an aliqupt of the methanol extract. Quantification of PFOS is accomplishedby liquid chromatography/tandem mass spectrometry( L c I M S / M S ) analysisusing selected readtion monitoring,(SM). ', I For this method the LOQ is 10 nglg (parts-per-billion). .This is based on stydiks conducted with egg membrarie, albumen, and yolk control samples during method development. t . I i I I ! I I . 1 1 rr .CentreAnalytical Laboratories. Inc. Study #0I23-015 .. Exygen Research ! .: Page 6 I ! Page 14 of 39 . I .. . ... .. ...- ... , c I Centre Method No: OOM-023-015 2. EXPERIMENTALCOMPOUNDS '. I .. The molecular structyreof PFOd is given below: I PFOS Molecular weight: 499 (CsF17S03-7 Chemical Name : Pe:rfluorooctanesulfonate W A C name :1-Octaneziulfonicacid,1,1,2,2,3,3,4,4,55,6,6,7,7,8,8,8- .. heptadecaifluoro-potassium salt , CAS # : 27'95-39-3 I I - I Note: The n e u d molecule and standard f o F which PFOS (anion)is derived I I from is perfluorooctanesulfonatepotassium salt [CSFI~SO~(Km]olecular ! weight 538). . .3. CHEMICAIS.&~ SUPPLIES . . 3.1. CHEMICALS - . . c 't' .. Chemical . . Grade Source CatalogNo. ' Carbon . 1201400 Supelco 572 10-U - - Methanol (Meow Ammonium Acetate HPLC . (VWR) J . T . B e e r fi9093-2 Reagent Aldrich Cher@cal 111-87-5 1 I Water Type I Centre i Vype I water = electrical resistivity,.minimum of 16.67MQ-cm at 25"C, from a I t Labconcow waterprg workstation, bged'on ASTM classification) .. .. - 3.2. STANDAkDS Standard Grade Test Control . Source . I Reference Number PFOS , Analytical TCR-000 E746 3M Environmental Laboratory, Si. Paul, h4N , ' Centre AnalyticalLabontcniu.Inc. Study # 023-015 ' Page 7 Y Exygen Research II Page 15of39 . I Il1 . iH '1 1 II II iI- ' IIII III I III Y .. i .. .. . .- ... . . L Centre Method No: OOM-023-015 3.3. EQULPP~EANMT)S U P P ~ S ' EQUIPMENT . SOURCE Balance, 5 place analytical Mettler Balance, 1place top-loading Mini Bead Beater-8 Wrist-action shaker Mettler Bio Spec Products : Burrell .. - Bench-top centrifuge Minicentrifuge -1201 50 mL disposable polypropylene centrifuge tubes IEC VWR VWR Stainless steel beads (cat # 11079) Bio Spec Products , Micro-centrifuge tubes VWR Disposable pipettes, test tubes etc. VWR 15-mL disposable polypropylene centrifuge tubes VWR Whamanm Anotopm Filter (cat # 6809-1022) VWR ' . I* . 2-mL E p p e n d o P microcentrifugetubes (cat# 22- 'VWR j 36-335-2) 8 . 2-mL clear HPLC vial kit (cat # 5181-3400) HP Standardlab equipment (class A pipettes'and volumetric flasks,graduatedcylinders,etc.) LC/MS/MS and HPLC!systems ASdescribedin . Section4.4.1. :. .. 1. In order to avoid contamination, the use of disposable labware is c highly recommended (containers, tubes, pipettes, etc.). 9 2. 'THePfLloCn voi-raltecfalposn,-slihnoeudldcnoonttabieneursseodr. equipment, . including teflo.n-lin. ed. I 4. It is necessrq to check the solvents (methanol) for the presence of ' contaminants by LC/MS/Ms before use. Certain lot numbers have been found to be'unsuitable for use. 5. . Use disposable rhicnipipettes or pipettes to aliquot standard solutions I and when preparing standards and samples for extraction. 6. .Equivalent :materials may be.substituted for those specified in this method. However, the use' of carbon from Supelco is strongly . recommended 3.4. SOLUTIONS .- i. 50 mM ammonium acetate solution: Dissolve 3.85 g of ammonium I acetate in 1L of ASTM w e I water. Store in an appropriate glass bottle at room tempcxature for up to 1 year. 2. 2 m M ammonium acetate solution: Dilute 40 of the 50 & ' . &onium acetate solution in a liter of ASTM type I wate;, for mobile .. Centre Analytical Labontorics, Inc. !Study # 023-015 . Pa& 8 Exygen Research Page 16 of 39 . I. I Ii . 1 I II 1 I I I rl ji *I I i I t \ I .' Ilhl .. . I Centre Method No: OOM-023-015 ' S phase A. Store: in an appropriate glass bottle at room tempexhre for up to ltyear. m: I The voluines shown are provided for guidance; alternative volumes! 1. may be prepared. I i'- 2, p I 3.5. TION ON OF STOCK, FORTIFICATIOANND, C A ~ Z B ~ T I O N SOLUTIONS , L L I Analytical stkdards an: prepared for two purposes. They are used to fortify untreated simples in order io determine analytical recovery and to calibrate the response oithe detectorused in the analysis. The analyst may vary the absolute volumes of the standards as long as the correct proportions of solute to solventare maintained. The solutions cited below are given as an.example; alternative concentrations may be prepared if needed. - 3.5.1. Stock Solutbn &pare stock solution of PEOS. at 100 pg/mL by weighing out 10.0 mg of analyticdstandard (corrected for percent salt). Adjust final volume to 100 mL with methanol in a 100-mL volumetric flask. Store this stock soiution (in 125-mL LDPE bottles) in a refrigerator at 2C to 6OC for a maximum period . of 6 mon,bs from the date of preparation. . -. 3.5.2. Fortij7catio.hSolutions a. 1.0 u&nL FortijScation Solution - Pipette 1.0 mL of the 100 p g / k stock . solution into a 100 mL. volumetric flask. Bring up to. volume with-' methanol. . b. . O ( ) i t i c a t i o n Solution - Pipette 10.0 d of the'1.0 pg/d fortification solution.into a IOO-mL volumetric flask and 6ring up to volume with me'thanol.. C. 0.01 u p / d Fortification Solution - Pipette 10.0 mL of the.0.1 p g / d fortificiition solution into a 100-d volumetric flask and bring up to volume with methanol. *. I , Store-all fortification standard solutions (in 125-mL LDPE bottles) in a refrigerator at 2C to 6C for a maximum period of 6 months from the date 1 .of preparation. 3.5.3. Calibration Standatdr Prepare six LCM3,iMS calibration standards in methanol via dilution of the - 0.1 p g / d and 0.01 pg//mLfortification so~utions. Centre Analytical Labor&ories,Inc. Study # 023-015 Page 9 . _ 1 Exygen Research Page 17 of 39 1 . Ill I I I 1 I I I i il J j rl I IH ll . IHM .. . .. I Centre Method No: OOM-023-015 vo. 1 ,o. 1 I 0.01 0.01 0.01 2 100 0.002 1 100 0.001 5 100 0.0005 1 100 0.0001 0.5 100 0.00005 Store all calibration Standard solutions (in 125-mL LDPE bottles) in a refrigeratorat 2C to 6C for a maximum period of 6 months from the date of preparation. 4. METHOD -4.1.'n o w DIAGRAM . . The flow diagram of the. method is given below, followed by a detailed descriptionof each step. . L e 'Weigh 1g of matrix (0.-lgfor membrane), Fortify if needed - 1. .. . Extract withMe'OH ~ 3. c C:arbon clean up (except membrane) L Filter . J Dilution ,. Lc/MSIM4s analysis I 4.i. SAMPLE PROCESSING -All samples are received frozen and will be kept frozen.@elow-10 "C)until time of the extraction. 4.3..SAMPLEEXTRAC~ION - NOTE: All egg sample masces were separated prior to arrival at Centre. . Z' Centre Analytical Lbontorics. Inc. Study # 023-015 Page 10 Exygen Research Page 18 of 39 I Y ! 1 I j. IQ .- I I d I i a i II .. . . _...-I-.-. .-.. . - 'I Centre Method No: 00M-023-015: 4.3.1 Egg Membrane i' . l a. Allow sample to thaw. I I b. Weigh 0.1 g (+ 0.005g) of sample into a 2 - a EppendorTM tube. Record f\' the weight to the nearest 0.0001g. Fortify untreated control samples at this point for determinationof method recovery. I I C. Add 1 IILof MeOH and three stainless steel beads, niplace lid tightly and. - homogenize with bead beater set at position 7 (-2500 rpm) for 5 minutes. Centrifuge the tubes with mini-centrifuge at 2,000 $m for 2,minUtes,' I then carefully transfer supematant to a new 2-mL-EppendorPM tube, I filtering with Whatmanm AnOtopm 10 filter if necessary. , d. Mi aaknega05.4Xmd~iloutfimonetbhyantroalnussfimng-hdgisp0.o1samblLemoficfrioltpraipteetttoesH(1P0L0C-2v0ia0lps~a)n.d. il ' e. Stom the rest of the extract in a refrigerator at approximately 2C to 6C. I for future re-dilution or re-injection. I 4.3.2. .Egg Yolk a i d Albumen , a Alloy sample to thaw. .. b. Weigh 1.0 g (2 0.05g) of sample into a 50-mL disposable polypropylene centrifuge tube. Record the weight to the nearest 0.0001g. Fortify untreated control samples at this point for .deterniination of method: recovery. C. Add 25 shaker f mL or 15 - of MeOH, replace lid tightly. minutes. Centrifuge tubes at and st&e 2,000 rpm -on a wrist-action for 10 minutes.. 1 d. Transfer about 5 mL of extract into a 15-mL disposable polypropylene . centrifuge tube, add 0.5 g cai-bon. replace lid tightly, arjd shake by hand for about 10 seconds. - e. Let the tubes sit for 2 minutes, Carefullytransfer -2.0 mL, of the sample , into a 1 0 - d . disposable syringe barrel connected to a Whatmanm . Anotopm 10 filter. Filter SWple into two HPLC viis, one for injection . and one for storage in a refrigeratorat approximately2C to 6C for future =-dilution or re-injection. Centre Analyticid Laboratories, Inc. !Study # 023-015 .. ! .. .. Page 11 i . I Q Exygen Research Page 19 of 39 . . I . .. S Centre Method No: OOM-023-015 II ; I i I II I ;I.i II 1 I I I j I . Mass Spec: I p~ sCIEX API 3000,Biomolecular Mass Analyzer Interface: . S ( X XTurbolon SprayLiquid IntroductisnInterface i. Zarvard infusion pump ; ! Computer. ' Power Macintosh G3 softwarc: . . ~ PI: Sciexhalyst 1.1 Windows NT HPLC: Hlewlett Packard (HP) Series 1100 I !b. HP Quat Pump. HP Vacuum Degasser HP Autosampler . I HP Column Oven . c . i HPLC Column: Genesis Cg (Jones Chromatograihy), 2.1 mm x 50 F , 4p . ColumnTemp.: 3!i0 C ., biection Vol.: 10pL Mobile Phase (A): 2 &AImmonium Acetate in ASTMrype I water Mobile Phase (B): Methanol . Flow Rate: 0.3 d m i n . ,w 9bA 0 60 . 1.0 0 7.0 0 1.5 40 . 11.0 40 - % B 40 100 100 60 . . 60 : . :.c . . p ,. [: t -1 !. It may .be necessary to adjust the HPLC gradient in order to optimize instrument performance. Columns with different dimensions (e,g., 2.1 mm x 4[, 30 mm) and columns from differentmanufacturers,(Keystone Betasil CIe8tc.) ! can be used, provided equivalent chromatographyis obtained. .. *- Ions monitored Approximate ' Analvte PFQS . Mode negative + Transition Monitored 499 99 Retention Time (min) 4.20 - ., - . On a day-to-day basis, the retention times may vary slightly depending-on the ' batch of mobile phase, etc. centre Analytical Laboratories,Inc. Study # 023-015 Page 12 . I 1 Exygen Research e Page 20 of 39 I" - .~. I . . . . .. I Centre Method No: OOM-023.015 . III I I 4.4.2.'Example Tune File Parameters I The following values are provided as 8n example. Actual values may vary I I from instrument to instrument. A h ,these values may be changed from time I1 to time in order to optimize for greatest`sensitivity. ' The mass spectrometer is tuned using a 0.5pghL PFOS solution,prepared via 1 I dilution of the stock solution in methanol. The solution is infused (using a `T'connector) at 10 W m i n into a 0.2 mUmin stream of mobile phase consisting of 40% methanol and 60% 2 mM ammonium acetate. The analytes are initially tunqd for the parent ion and then tuned for the product ion. Once III the instrument is tuned, the optimized parameters are saved as a "tune file". !.I This tune fileis then used during routine analysis. The tuning procedure may I. be repeated as'necessq to ensure Optimal Sensitivity. I .. r I I I Controls Set IS-Iodpray 46TO . OR-Orifice -6 1.O RNG-FocusRing -270.0 QO-Quad 0 Rod Offset 10.0 144-Inter quad 1lens 9.3 STBtubbies- 15.0 RO1-Quad1 Rod Offset . 9.3 IQ2-Inter quad 2 lens 20.0 R02-Quad 2 rod offset 84.0 . .c . ST3-Stubbies . 100.0 R032.Quad 3 rod ol`fset 86.0 DF-CEM Deflection Plate 300.0 CEM-Channel Electron Multiplier 2400.0 i x Gas R>ws :NebulizerGas Curtain Gas Collisiorl Gas . . TISTemperature ~ . .-Set 1 .12 . 13 .4 350'C 3.4.3. Calibration ;Procedures a. Inject the same v,olume(between 10 to 20 &) of each calibration standard . (prepared in MeOH) into the LC/MS/MS. . b. Use linear, l/x weighted standard curves for quantification. Linear . stgdarcl curves are generated for each set by linear regression using the . Centre Analytical Laboratories. Inc.Sltudy#0I23-01s page` 13 1 Exygen Research Page 21 of 39 -. . i 1 i!I .' I i I i j i I I i i ! i I . - .. .. .-. .. . .. . . , L' . Centre Method No: 00M-023-015 appropriate sofiware system. Any cqbration standards fdling outside f , 30%. based on its calculated concentration, must be excluded from the calibration curv~:. However, the total number of calibration standards th; may be excluded must not exceed 30% of the total number of stand=& injected. c. The correlation coefficient (r) for ,calibration curves generated must be I' 20.9925 (220.985). If calibration results fall outside 'these limits, then appropriate steps should be taken to adjust instrument operation, and the relevant set of simples must be reanalyzed. ; I 4.4.4. SampleAnalysis i a. Inject the same volume used for the calibration standards (between IO to 25 pL)of each sample, fortification,control, etc. into the LC/MS/MS. b. Standards correspondingto at least Si.x concentrationsmust be included in I an analytical set. c. Inject an entire :ret of standards (six) at the beghing of the run and inject standards interspersed about every 3-10 samples. All sample injections must be bracketed by standard injections (see Section4.5). *. '1 d. Each set of samples analyzed (not to exceed 25) must include at least one reagent control (method blank). one ASTM Type I water blank, at least one matrix control, b d two matrix confrol samples fortified at known concentrations and carried through the procedure to verify recovery. .. e. All samples must be analyzed with duplicate injections. ':: . 'i .. - ,. Note: ansllysis performed -during method development included ' fortifications at 10,50 and 250 ndg (ppb) for the mdilyte. 1. 1 I f. The concentration of each sample; fortification,contiol, etc. is determined iI, from the.standard curve based on the peak area of the anaiyte in all standards injected during a .set. ' The standard responses must bracket responses of thr: residue found in the sample set. If necessary, dilute the samples &d re-:analyzeto give a fisponse within the standard curve range. , g. Fortifications that bracket the highest residue expected in each treated . sample Vjill be included with each sample set. If residues <are found . ' outside these limits, additional fortifications will be .included in a . subsequent sample'set to establish e a t method recoveries are available for the,analyteof interest at concentrationsexceeding those in treued samples. .. .. Centre Analytical Laboratories. Inc. Study # 023-015 .: Page 14 . Exygen Research Page22of39 . . ., c . I I Centre Method No: 00M-023-015 I h. Fortification recoveries &thin 60 to 130% are acceptable for fortifications at the LOQ level. Recoveries between 70 to 120% are acceptable f0.r fortifications at levels greater than $e LOQ. Failure to meet these criteria . requires an investigatioi Of cause and a full reanalysis of the affected 1P samples. j i. Samples in which no vaks are detected at the corresponding analyte retention times will be reported as ND (not detected). Samples in which peaks are detected at the kOITeSponding analyte retention times but are less than the lowest standard will be ported as NQ (not quantifiable). j. If samples are not loaded on the hstrument to be analyzed'theday they are extracted,samplesmust be stored.refrigeratedat approximately ZoCto ij0c until analysis and analyzed preferably within a week. Recoveries from' method development for all matrices can be found in Tables I-VI. .. 4.5. PERFoRMANcEc- . .. .. The f&wiig two crit:&a must be met before the initial analysis of samples, especially when using different instrumentation set-ups than those cited in this method. First Criterion- Inject a standird solution on the LCIMSIMS corresponding to:t h e estimated LOQ (10 ppb LOQ kequivalent to a standaid solution of 0.2 ng/mL) and obtain a signal to noise ratio Of at least 9:1 relative'to the reagent blank. If this criterion cannot be met; optimize change .instrument operating parameters. - Second Criterion Inject a set of'standardsranging from at or below the LOQ, up to the highest concentra.tion leyef. Generate a calibration curve for theanalyteand I obtain a linear regression with a:co$icient of determination (r2)of at least 0.985 . . , for the analyte. Once: this criterion has been demonstrated, samples may be analyzed with standardsinterspersed. , Centre Analytical Laboratories,Inc.Study#0I23-015 .. Exygen Research . Page 15 Page 23 of 39 . .- .' ' ' -... - Centre Method NO:00M-023-015 L . III ; ,a 4.6. TIME REQUIRED FOR ANALYSIS 6 , A set of 14 samples can be taken through the extraction procedure in I approximately three hours by one person. The LCMSMS analysis (8-10 ...i Id i standards and 14 sample:;) will take approximately6 hours. I *! . ,$ 1 5. CALCULATIONS m .5.1 ANA~TEFOUND: Calculate the amount of analyte found (in ng/mL, based on pe& m a ) using he standard curve generated ;by the MacQuan ~ o f t w mp r o m using Equation 1. . Equationl: Anaiyte found ( n g / d ) = b e a k area - intercept) slope. 5.2 COMFONEN&TSI.K)UECONCENTRATION ., . , t. .: I . Determine the component residue concentrationusing Equation 2 .. Equation2: . .. Residue found (ng/g) = (analyte found (nglmL) x DF x Fv (IT&)) sample weight (g) Where DF= dilution factor and Fv = final volume a:nglg = ppb 1 5.3 PERCENTRECOVERY Calculate the peient recavery for samples fortified with known amounts of analytes prior to extraction, from Equation 3. .-I - Equation3: . I.- (nglg found - averageng/g found in control) ! .. .. Recovery (%) = @gadded . XlOO , c e m Analytical Laboratories,I'm. StudyIt 023-015 Exygen Research Page 16 ! .f ' .. Page 24 of 39 . I Im Ill I1 i. '. ,II. . L .- . .. . I ' Centre Method No: OOM-023-013 i 6. SAFETY * I, I' There are no unusual hazards associated With this method. The analyst should 11 t' read the material safety thta sheets for dl Tagents before performing this method Normal laboratory precautions should be taken. .I I 4 L 1 .. b . I .I I .. c .. I .. Centre Analytical Labontories,Inc..Study# 023-015 i. Exygen Research Page 17 Page 25 of 39 I I lllll - 1 .I . IH ' '. .. I I Centre Method No: 00M-023-015 . t i . I I . .. 4' TABLES rl I a . .. fI. .. I '. i .,. . I j. I 1' f f ! .. c Centre Analytical Laboratories, Inc. Si:udy # 023-015 Exygen Research . I .. Page 18 . Page26of39 . in I IU I I I' 1 -I - I .. Centre Method No: OOM-023-015 Table I: Summary of Recoveries for PFOS in Quail Egg Membrane Sample ' 0003798 Matrix Blank A F o i Level' (ppb) 0 0003798 Matrix Blank I 0 0003798 Matrix Blank C 0 0003798 Spk A 10 0003798 Spk B 10 0003798 Spk C 10 0003798 Spk D 50 0003798 Spk E 50 0003798 Spk F 50 0003798 Spk G 250 0003798 Spk H 250 0003798 Spk I 250 AVERAGE STANDARD DEVIATION RELATIVE STANDARD DEVIATION %Recovery NA NA NA 88 95 92 92 95 96 93 95 93 93 2 8 . 3 Table II: Summary of Recoveries for PFOS in Mallard Egg Membrane - _. Sample Fort Level % Recovej (ppb) 0003802 Matrix Bla& A 0 NA 0003802MatrixBlankB . 0 NA 0003802 Matrix Blank C ' 0 NA 0003802 Spk A 10 106 0003802 Spk B . 10 122 0003802 Spk C 10. 106 0003802 spk D 50 96 0003802 Spk E 50 96 0003802 Splc F 50 90 0003802 Spk G 250 93 0003802 Spk H 250 92 0003802 Spk I . 250 93 AVERAGE: 99 . STANDARDDEVIATION: 10 RELAT[VE STANDARDDEVIATION. 10 NA = Not Applicable . . I. ! ' I) ! j .. ' C .. . : ! . I 'I 1 .; I . Centre Analytical Laboratories. Inc. Study 11 023-015 Exygen Research Page 1.9 Page27 of 39 . 1 I i II . a Centre Method No: 00M-023-015 . Table,III: Summary of Recoveries :orPFOS in Quail Egg Yolk Sample 0003795 Matrix Blank A 0003795 Matrix Blank B 0003795 Matrix Blank C 0003795 Spk A 0003795 Spk B 0003795 Spk C 0003795 Spk D GUO3795 Spk E 0003795 Spk F 0003795 SRk G 0003795 Spk H Fort. Level I . * (n&) o 0 0 10 . 10 ' 10 50 I ' 50 50 I ' ' 250 . 250 9b R e ~ ~ v e r y a I ! NA NA NA 69. 68, 70 72 80 83 85 ' 89 0003795 Spk I 250 88 AVERAGE: 7.8- .STANDARDDEVIATION RELAmrE STANDARDDEVIATION -9 11 Table IV: Summary of Receveries for PFOS in Mallard Egg Yolk Sample - 0003799 Matrix Blank A . 0003799 ~ a t r i xBlank B , 0003799 Matrix Blank C 0003799Spk.A . 0003799 Spk B 0003799 Spk C 0003799 Spk D 0003799 SpkE 00037.99 Spk F 0003799 Spk G 0003799 Spk H 0003799 Spk .I Fort Level (nglg) 0 0. 0 ' 10 10 . 10 50 * 50 50 250 250 250 AVERAGE: % Recovery NA NA NA 83 82 1OQ 85 . 8 8 ~. 90 87. 85 ' 88 88' STANDARD DEVIATION 5- . aUm/'ESTANDARDDEVIATION: . 6 .. .- ! NA = Not Applicable .. : I .. . Centre Analytical Labontories, Inc. Study # 023-015 Page20 . '. I Exygen Research Page 28 of 39 I IN i ! .. I Centre Method No: 00M-023-015 . . Table V: Summary of Recoveries for PFOS in Quail Egg Albumen . . Sample I Fort. Lcvel 46 Recovery ' I - I (ppb) 0003196Matrix Blank A 0 NA ! 0003796 Matrix Blank B 0 NA j; 0003796 Matrix Blqnk C 0 NA I a03796 Spk A 10 79 I( v 3 7 9 6 Spk B 10 . 0003796 Spk C 10 93 88 - 0003796 Spk D 50 96 0003796 Spk E 50 95 0003796 Spk F 50 90 0003796 Spk G 250 . 97 0003796 Spk H .250 102 " 0003796 Spk I 250 AVERAGE: 102 94 . STANDARD DE'VIATION: 7 . REI.,AlWE STANDARD DEVIATION: 7 Table VI: Summary of Recolveriesfor PFOS in Mallard Egg Albumen Sample . -- Fort.Level (ppb)' ~ : 0003800MatrixBlankA ' 0 0003800 Matrix Blank B 0.. 0003800MatrixBlank C . 0 0003800 Spk A , ' 10 - 0003800SpkB 10 0003800 Spk C 10 - 0003800 Spk D 50 0003800Spk E 50 Ob03800 Spk F . 50 . 0003800 Spk G 250 0003800 Spk H 250 0003800 Spk I 250 .. AVERAGE: STANDARD DEVIATION: ' RELATIVE STANDApD DEVIATION: 46 Recovery NA NA NA ' . 93 85 85 96 100 100 . 98 102 . - 101 ' 96 7 7 . NA = Not Applicable .. Centre Analytical Labonton&, Inc. Study k 023-015 Exygen Research . ! Page 21 Page 29 of 39 . II II d 1I . .. ..--.- ---.-_.-. Centre Method No: OOM-O&-015 s . I FIGURES I I 4 ! I , f. 1, . C C N ~A~nCalytical Laboratories.INC.Study # 023-015 . Exygen Research Page 22 Page 30 of 39 . , , .. . - , ___________,____._._... .... . . .. '' - ' .- .---. -. .. -.--.-..-...---. ---- ----.-.__ _ ____ -. S . 6 ' Centre Method No: OOM-023-015 I Ii Figure 1: Repraentatiye Chromatogram of a Quail EggMembrane Control ! . 11 1luAk 0.000 OUO~I00 a:u:3r 111 lu 1 1.61 ; 1.11 III ! .. i ' Figure 2: Representative Chromatogram of a Mallard Egg Membrane Control .-. . . 11'1 ! 11 -1 II Centre AnalyticalLaboratories, IIIC.Study # 023-015 Exygen Research -Page 23 Page 31 of 39 . .-. ... - . III I Centre Method No: OOM-023-015 . Figure 3: Representative Chromatogram of a Quail Egg,Yolk Control ! I. m la P rn 1 ,la 1.n u 1.11 1 u t; II 1t.1 IK 7.11 dr 14 0.1 0.01 ' s.w 4.w 1.1) .n m Y UI ! .- - Figure 4: Representative Chromatolgram of a Mallard Egg Yolk Control t : II T : -' I Centre h l y t i c a l Laboratories, Inc:. Study # 023-015 Exygen Research Page 24 Page32of39 . . lllll Centre MethodNO:OOM-023-015 Figure 5: Representative Chromatogramof a Quail Egg Albumen'Control tn. U n Y w MI :1I 7 7 L 1 ! I! Ill1 I 1 Figure 6: Representative Chroma1:ogramof a Mallard Egg Albumen Control I u( I I ! . Centre Analytical Laboratories, Inc. Study # 023-015 ., . Exygen Research Page 25 Page 33 of 39 I1 I . Centre Method No: 00M-023-015 S' 1111 Fipre 7: Representative Chromatogram of a Quail EggMembrane Control Fortified at 10 ng/g (ppb) . 11 I I .- _. 'Figure8: Representative Chromatogram of a Mallard Egg Membrane Control Fortified at 10.0 ng/g (ppb) , .-- I I.6i 1.11 ;1 11.0 a u 1.10 mia 0.10 1.01 . 1.oa k.03 3.M L ru R i ui u( "iu . I ! c 2 .. 1 Centre Analytical Laboratories,Inc. Study # 023-015 .Exygen Research Page 26 Page34of39 c lllll Centre Method No: 00M-023-015 ; Figure 9: Representative Chromatogram of a Quail Egg Yolk Control Fortified at 10.0 ng/g @pb) . . Il1 . I ' Figure 10: -RepresentativeChromatogram of a Mallard Egg Yolk Control Fortified at 10.0 nglg (p:pb) I II . .z .. .. lI. T1U IIN ' i 1-66 1.11 Y I . 1 10.I sac l.Il..Ln 8.20 0.81 ; u m ' w 1.00 . Y 4.00 1.00 (I( lo mI I . II IIII Centre Analytical Laboratories, Inc. Study # 023-015 Exygen Research ! . . .. Page 27 Page35 of39 . Ill I * ! Centre Method No: OOM-023-0151 b - Figure 11: Representative Chromatogram of a Quail Egg Albumen Control Fortified at 10.0 ng/g (ppb) ..I m I i I I i! . , I in i ii 1I ! I I u u u u I I I.! I ! - ! : Figure 12: Representative Chromatogram of a Mallard Egg Albumen Control Fortified at 10.0 ng/g (p:pb) I -. . I -1 I : I' 1 I ! I I It Centre Analytical Laboratories. Inc. Study #,02.3-015 . . Exygen Research , Page 28 Page 36 of 39 1 Lipovitellin, Phosvitin, a n e w Low from Chicke9n6 a[1n9d6J0a]pandesSetiQfauniaiiiei t gaIg.,:: Density g Lipo'pr.otein (VLDL) 5 . Isolation - d ! (May, 1994) * I 1) Break open egg, separate yolk, and roll yolk on a moist paper towel to remove adhering albumen. 2) Puncture yolk membrane and let yolk drain into a graduated cylinder, 3) Dilute 1 volume of egg yolk with 2 volumes of a solution containing 0.67 M MgS04, 1 mM phenylmethanesulfonylfluoride(PMSF), and 2'pM leupeptin. II 4) Cover cylinder tightly with Parafilm@Mand mix well by gently inverting several times. 5) Using a 20 gauge needle arid 12 cc syringe, transfer the suspension to Beckman polyallomer Quick-Seal@tubes (tube size will depend on amount of yolk prepared and rotors available). IIIII 6 ) Seal tubes, place into appropriate rotor, and centrifuge at 200,000 x g at 4 O C .for 2 4 hours. 7 ) Following centrifugation, 4 layers will be evident in the tubes (see diagram at right): A, a firm layer of yellow gel (VLDL); B, a clear colorless solution; C, a viscous yellow solution grading to a firm A- IIII pellet at the bottom; D, a fluffy yellow suspension (VLDL). Layers B and C constitute the high density fraction (HDF) and layer A and the suspended material in D constitute the (very) low density fraction. C 8 ) Using a 20 gauge needle and 12 cc syringe, make t w o punctures in the r top of the tube and withdraw layer D as well as several milliliters below the level of layer A until layer B is reached. 9) With a scalpel, cut the tube above the level of the remaining liquid. The yellow upper pellet of the tube (VLDL) is then redissolved in a solution containing 20 mM Tris-HCI (pH 81, 150 mM NaCI, 0.2 mM EDTA, 1 mM PMSF, and 5 pM leupeptin. The lower pellet (high density . fraction, HDF; Layer C) should be gently washed with, and then I resuspended in, a solution containing 0.45 M MgS04, 1 mM PMSF, 'Ill Exygen Research Page 37 of 39 c 2 . and 2 pM leupeptin. Both VLDL and' HDF solutions are then centrifuged at 200,000 x g at 4 "C for 16 hours. 10) Following centrifugation of the VLDL solution, the upper pellet (VLDL) is . . re-dissolved in a minimal amount of 20 mM Tris-HCI (pH 8), 150 mM NaCI, 0.2 mM EDTA, 1 rriM PMSF, and 5'vM leupeptin, filtered (0.45 pM), sodium azide added to a final concentration of 1 mM (i.e., dilute stock solution 1000 XI,aliquoted, and stored at 4 "C. All of the VLDL preparation is now completed. The lower pellet (Layer C) of the HDF tube is first re-dissolved in a solution Of 0.45 M MgS04, 1 mM PMSF, and 2 pM leupeptin. Then, two volumes of cold "e-pure" water are added to the HDF solution dropwise, with stirring, at 4 "C (thus, MgS04 concentration is now 0.15 MI. The solution is then left standing (without stirring) at 4 "C overnight. 11) On the following morning, is yellow gelatinous precipitate should be adhered to the bottom of the flask. Decant (and save) the supernate (see step 12), then dissolve the precipitate in a solution of 0.4 M MgS04, 1 mM PMSF, and 2 pM leupeptin. Add one volume of cold "e-pure" water dropwise (thus solution is diluted to 0.2M MgS04) and let stand overnight (without stirring) a t 4 "C. On the following morning, the precipitate I(phosvitin1is recovered by centrifugation at 106,000 x g at 4 "C for 1 hour and the resulting pellet is dissolved in buffer containing 1 M NaCI, 5 m M Tris-HCI (pH 7.81, 1 mM PMSF, 2 pM leupeptin, and sodiurn azide added to a final concentration of 1 mM (i.e., dilute stock solution 1000 XI. Aliquot and store at 4 "C. 12) The "supernate" (0.15 M IlrlgSO4; see step 11) should be decanted, diluted with two volumes of cold "e-pure" water (final concentration of 0.05 M M g S 0 4 ) dropwise with stirring at 4 " C , and allowed to stand overnight (without stirring) at 4 "C. The resulting white precipitate (lipovitellin) is then recovered by centrifugation at 106,000 x g at 4 "C for 1 hour and dissolved in buffer containing 1 M NaCI, 5 mM Tris-HCI (pH 7.81, 1 mM PMSF, and 2 pM leupeptin, and sodium azide added to a final concentration of 1 mM (i.e., dilute stock solution 1000x). A final protein concentration of 8-10 mglmL is desired. '/I IIIIN I1 1I llIY Exygen Research Ill - iI Page38of39 . d Ill Exygen Research Page39of39 .