Frontiers in Chemistry (May 2021)
Global-Scale Metabolomic Profiling of Human Hair for Simultaneous Monitoring of Endogenous Metabolome, Short- and Long-Term Exposome
Abstract
Hair is a unique biological matrix that adsorbs short-term exposures (e. g., environmental contaminants and personal care products) on its surface and also embeds endogenous metabolites and long-term exposures in its matrix. In this work, we developed an untargeted metabolomics workflow to profile both temporal exposure chemicals and endogenous metabolites in the same hair sample. This analytical workflow begins with the extraction of short-term exposures from hair surfaces through washing. Further development of mechanical homogenization extracts endogenous metabolites and long-term exposures from the cleaned hair. Both solutions of hair wash and hair extract were analyzed using ultra-high-performance liquid chromatography-high-resolution mass spectrometry (UHPLC-HRMS)-based metabolomics for global-scale metabolic profiling. After analysis, raw data were processed using bioinformatic programs recently developed specifically for exposome research. Using optimized experimental conditions, we detected a total of 10,005 and 9,584 metabolic features from hair wash and extraction samples, respectively. Among them, 274 and 276 features can be definitively confirmed by MS2 spectral matching against spectral library, and an additional 3,356 and 3,079 features were tentatively confirmed as biotransformation metabolites. To demonstrate the performance of our hair metabolomics, we collected hair samples from three female volunteers and tested their hair metabolic changes before and after a 2-day exposure exercise. Our results show that 645 features from wash and 89 features from extract were significantly changed from the 2-day exposure. Altogether, this work provides a novel analytical approach to study the hair metabolome and exposome at a global scale, which can be implemented in a wide range of biological applications for a deeper understanding of the impact of environmental and genetic factors on human health.
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