Chemistry to Community: Development and Implementation of a GC-MS/MS Method for Exposure Assessment and Evaluation of Community-Engaged Research in the Michigan PBB Research Registry Restricted; Files Only

Marder, M. Elizabeth (2015)

Permanent URL: https://etd.library.emory.edu/concern/etds/fb494909t?locale=en
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Abstract

Polybrominated biphenyls (PBBs) are first generation brominated flame retardants, which, along with their replacements, are considered contaminants of concern due to their persistence and toxicity. In 1973, the accidental introduction of FireMaster flame retardant into the Michigan food chain resulted in widespread exposure to PBBs and prompted the establishment of the Michigan PBB Registry to evaluate long-term human health effects. This multigenerational cohort of approximately 5,000 individuals includes those exposed occupationally or by consuming contaminated food and subsequent generations who may have been exposed in utero or through breastfeeding. This cohort has been maintained for nearly forty years, and findings to date associate exposure with a variety of health outcomes. However, over time, different analytical approaches involving different standard materials and instrumentation have been used to assess exposure, affecting validity of direct comparisons of measurements across time periods. Moreover, prior to the current study, the most recent assessment of PBB body burden in this population was conducted over twenty years ago. A critical component of current and ongoing community-engaged research is accurate exposure assessment; this necessitated the development of a highly sensitive and selective analytical method capable of quantifying 11 PBBs and 4 polychlorinated biphenyls (PCBs) utilizing gas chromatography-tandem mass spectrometry with isotope-dilution quantification. The method was validated using in-house fortified pooled human sera and standard reference material from the National Institute of Standards and Technology. Limits of detection were in the low pg/mL range (0.7-6.5 pg/mL) with good accuracies (84-119%) and precision (relative standard deviations <19%). This method was applied to sera from current study participants (2012-2015) and to archived serum analyzed previously for PBB-153 (1976-1993); PBB-153 concentrations are presented and discussed, with those for archived samples contrasted with originally reported concentrations to evaluate performance of earlier analytical approaches and determine the comparability of these exposure measurements. Additionally, community engagement is a significant component of PBB research, to an extent it merited evaluation. This evaluation, which included application of the National Institute of Environmental Health Sciences metrics for partnerships in environmental public health, characterized the benefits of community-engaged research and elucidated its importance in this research context.

Table of Contents

Chapter 1 Introduction and Background

1.1 The Michigan Contamination Incident

1.2 Polybrominated Biphenyls

1.3 The Michigan PBB Research Registry

1.4 Impetus for Analytical Method Development

1.5 Analytical Method Development: Considerations for Quantification of PBBs and Selection of Approach

1.6 References

Chapter 2 Quantification of Polybrominated and Polychlorinated Biphenyls in Human Matrices by Isotope-Dilution Gas Chromatography-Tandem Mass Spectrometry

2.1 Abstract

2.2 Introduction

2.3 Experimental

2.4 Results

2.5 Discussion

2.6 Conclusions

2.7 Funding

2.8 Acknowledgements

2.9 References

Chapter 3 Current Exposure to PBB-153 in the Michigan PBB Research Registry

3.1 Abstract

3.2 Introduction

3.3 Methods

3.4 Results

3.5 Discussion

3.6 Conclusion and Public Health Relevance

3.7 Funding

3.8 Acknowledgements

3.9 References

Chapter 4 Evaluation of Historic Measures of Polybrominated Biphenyl 153 Exposure in the Michigan PBB Research Registry

4.1 Abstract

4.2 Introduction

4.3 Methods

4.4 Results

4.5 Discussion

4.6 Conclusion

4.7 Funding

4.8 Acknowledgements

4.9 References

Chapter 5 Community-Engaged Research in the Michigan PBB Research Registry

5.1 Abstract

5.2 Introduction

5.3 Methods for Evaluation

5.4 Implementation

5.5 Discussion

5.6 Conclusion

5.7 Funding and Acknowledgments

5.8 References

Chapter 6 Appendix

6.1 Sample Collection and Processing

6.2 Instrumental Method for Quantification of Related Organohalogens

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