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Method optimization for detection of arsenolipids in standard reference materials and seafood using HPLC-ICP-MS and HPLC-ESI-MS, and bioavailability of ASFA362 through In Vivo st

Year: 2024
Type: dissertation
Abstract: Arsenolipids, lipid-soluble arsenic compounds found in marine organisms, pose potential health risks due to their toxicity. However, research on their toxicological impacts is limited, partly due to challenges in separating and identifying organoarsenic compounds in complex biological matrices and the absence of certified standard reference materials (SRMs). This study addresses these challenges by developing a workflow for identifying arsenolipids in biological samples, and harmonizing extraction and data processing methods across studies. Arsenolipids were extracted from three marine SRMs—Hijiki seaweed (CRM 7405-b), Dogfish liver (DOLT-5), and Tuna fish (BCR-627)—using hexane and dichloromethane (DCM)/methanol (MeOH). The extracts were analyzed via reverse-phase high-performance liquid chromatography-inductively coupled plasma mass spectrometry (LC-ICPMS) and LC coupled with electrospray ionization quadrupole time-of-flight mass spectrometry (LC-ESI-QTOF-MS). A workflow was developed by first populating a precursor library for arsenolipids to facilitate the analysis. The study identified various arsenolipids, including arseno-fatty acids (AsFAs), arsenohydrocarbons (AsHCs), and arsenosugar phospholipids (AsSugPLs). Notably, AsHC332 and AsFA502 were consistently detected across all SRMs, highlighting these as potential candiadtes for synthesis and toxicity analysis. Applying this workflow, the arsenolipid content in seventeen canned tuna samples and nine salmon samples from local markets in Lubbock, Texas, was analyzed. Tuna showed a higher total arsenic concentration (4.73 ± 4.65 mg/kg) compared to salmon (0.92 ± 0.44 mg/kg), with arsenolipids ranging from 0.34% to 24.67% and 0.01% to 24.52% of the total arsenic content, respectively. Key arsenolipids identified in tuna included AsFA362, AsHC332, AsHC358, and AsHC404, while salmon contained AsHC360, AsHC332, and AsHC404. The third study further investigated the bioavailability of AsFA362 in mice at 400 µg/L concentrations, similar to levels in marine biota. Analysis of total arsenic in urine and feces indicated a mean recovery rate of 4.59 ± 2.03%, with over 90% of AsFA362 retained in organs, suggesting high bioavailability. In conclusion, this dissertation advances the analytical methodology for arsenolipid identification in marine biota and provides significant insights into the bioavailability and retention of AsFA362 in mice. These findings underscore the potential health risks associated with arsenolipid exposure from seafood consumption, highlighting the necessity for further toxicological research and the establishment of safe exposure limits. This is crucial for informing regulatory policies and protecting public health.
Language: English
Open Access status: green
OpenAlex ID: W7049284824
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