Nontargeted Biomonitoring of Halogenated Organic Compounds in Two Ecotypes of Bottlenose Dolphins (Tursiops truncatus) from the Southern California Bight
Abstract:Targeted
environmental monitoring reveals contamination by known
chemicals, but may exclude potentially pervasive but unknown compounds.
Marine mammals are sentinels of persistent and bioaccumulative contaminants
due to their longevity and high trophic position. Using nontargeted
analysis, we constructed a mass spectral library of 327 persistent
and bioaccumulative compounds identified in blubber from two ecotypes
of common bottlenose dolphins (Tursiops truncatus) sampled in the Southern California Bight. This… Show more
“…Higher levels than the ones reported here were found in bottlenose dolphins from the Pacific Ocean 12 and its contributions were also higher than PBDEs in bottlenose dolphins from Southern California Bight. 29,30 In addition, similar values of MeO-PBDEs were found in blubber biopsies of common (240 ng/g lw), pilot (312 ng/g lw) and bottlenose (628 ng/g lw) from southern European waters. 57 Differences between the levels reported worldwide is affected by the different HNPs producers existing in each area, number of monitored congeners, and also by the different preys available, since dietary uptake is the main bioaccumulation route of these compounds.…”
Halogenated natural products (MHC-1, TriBHD, TetraBHD, MeO-PBDEs, Q1, and related PMBPs) and halogenated flame retardants (PBDEs, HBB, Dec 602, Dec 603, and DP) in blubber and brain are reported from five Alboran Sea delphinids (Spain). Both HNPs and HFRs were detected in brain, implying that they are able to surpass the blood-brain barrier and reach the brain, which represents a new finding for some compounds, such as Q1 and PMBPs, MHC-1, TriBHD, TetraBHD, or Dec 603. Moreover, some compounds (TetraBHD, BDE-153, or HBB) presented higher levels in brain than in blubber. This study evidence the high concentrations of HNPs in the marine environment, especially in top predators. It shows the importance of further monitoring these natural compounds and evaluating their potential toxicity, when most studies focus on anthropogenic compounds only. While no bioaccumulation was found for ∑HNPs, ∑HFRs increased significantly with body size for both common and striped dolphins. Studies evaluating BBB permeation mechanisms of these compounds together with their potential neurotoxic effects in dolphins are recommended.
“…Higher levels than the ones reported here were found in bottlenose dolphins from the Pacific Ocean 12 and its contributions were also higher than PBDEs in bottlenose dolphins from Southern California Bight. 29,30 In addition, similar values of MeO-PBDEs were found in blubber biopsies of common (240 ng/g lw), pilot (312 ng/g lw) and bottlenose (628 ng/g lw) from southern European waters. 57 Differences between the levels reported worldwide is affected by the different HNPs producers existing in each area, number of monitored congeners, and also by the different preys available, since dietary uptake is the main bioaccumulation route of these compounds.…”
Halogenated natural products (MHC-1, TriBHD, TetraBHD, MeO-PBDEs, Q1, and related PMBPs) and halogenated flame retardants (PBDEs, HBB, Dec 602, Dec 603, and DP) in blubber and brain are reported from five Alboran Sea delphinids (Spain). Both HNPs and HFRs were detected in brain, implying that they are able to surpass the blood-brain barrier and reach the brain, which represents a new finding for some compounds, such as Q1 and PMBPs, MHC-1, TriBHD, TetraBHD, or Dec 603. Moreover, some compounds (TetraBHD, BDE-153, or HBB) presented higher levels in brain than in blubber. This study evidence the high concentrations of HNPs in the marine environment, especially in top predators. It shows the importance of further monitoring these natural compounds and evaluating their potential toxicity, when most studies focus on anthropogenic compounds only. While no bioaccumulation was found for ∑HNPs, ∑HFRs increased significantly with body size for both common and striped dolphins. Studies evaluating BBB permeation mechanisms of these compounds together with their potential neurotoxic effects in dolphins are recommended.
“…The extracts were spiked with 13 C-PCB-153, BDE-77, BDE-166 and 6-FBDE-47 as internal standards prior to automated gel permeation chromatography (24 g BioBeads S-X3 eluted with 1:1 ethyl acetate/cyclohexane at a flow rate of 5 mL/min), as described previously 16,17 . The eluent fraction between 8.5 and 20.5 min was collected and evaporated to 1 mL under N 2 gas, and the GPC purification step was repeated to remove residual lipids.…”
Section: Methodsmentioning
confidence: 99%
“…2) The fragmentation pattern must indicate a halogenated loss (either bromine and/or chlorine). A reference data processing method was created from the 150 peaks and used to search the remaining three samples 17 . The allowed retention time deviation, set based on the modulation time, was ± 3.5 s in the 1st dimension and ± 0.05 s in the 2nd dimension.…”
Section: Methodsmentioning
confidence: 99%
“…This value was then divided by the mass of extracted lipid for each sample to give the normalized relative abundance. Due to the unavailability of synthetic standards for most of compounds, the normalized abundances are considered semi-quantitative 17 . Variation between the normalized abundance profiles of the Californian and Brazilian dolphins was investigated by principal component analysis (PCA) using R 24 function prcomp and visualized using function biplot .…”
Section: Methodsmentioning
confidence: 99%
“…Due to its top predator status, life history, and presence near densely populated areas, cetaceans have been studied via targeted analyses 15 , and more recently using NTA. Hoh and coworkers identified a total of 270 halogenated organic compounds (HOCs) in a blubber sample of a common dolphin ( Delphinus delphis ) stranded in the NW Atlantic 16 ; a second study using the same methodology reported 327 HOCs in the blubber of bottlenose dolphins ( T. truncates) frequenting the southern California coast in the NE Pacific 17 . Comparison of the HOCs catalogued in these geographically disparate studies revealed differences in the relative distribution of anthropogenic contaminants, halogenated natural products, and unknown HOCs.…”
To catalog the diversity and abundance of halogenated organic compounds (HOCs) accumulating in high trophic marine species from the southwestern Atlantic Ocean, tissue from bottlenose dolphins (Tursiops truncatus) stranded or incidentally captured along the coast of Rio de Janeiro, Brazil, were analyzed by a non-targeted approach based on GC×GC/TOF-MS. A total of 158 individual HOCs from 32 different structural classes were detected in the blubber of 4 adult male T. truncatus. Nearly 90 percent of the detected compounds are not routinely monitored in the environment. DDT-related and mirex/dechlorane-related compounds were the most abundant classes of anthropogenic origin. Methoxy-brominated diphenyl ethers and chlorinated methyl- and dimethyl bipyrroles (MBPs and DMBPs) were the most abundant natural products. Reported for the first time in southwestern Atlantic cetaceans and in contrast to North American marine mammals, chlorinated MBPs and DMBPs were more diverse and abundant than their brominated and/or mixed halogenated counterparts. HOC profiles in coastal T. tursiops from Brazil and California revealed a distinct difference, with a higher abundance of mirex/dechloranes and chlorinated bipyrroles in the Brazilian dolphins. Thirty-six percent of the detected HOCs had an unknown structure. These results suggest broad geographical differences in the patterns of bioaccumulative chemicals found in the marine environment, and indicate the need to develop more complete catalogs of HOCs from various marine environments.
Objectives
Tris(4‐chlorophenyl) methane (TCPM) and tris(4‐chlorophenyl)methanol (TCPMOH) are anthropogenic environmental contaminants believed to be manufacturing byproducts of the organochlorine pesticide dichlorodiphenyltrichloroethane (DDT) due to environmental co‐occurrence. TCPM and TCPMOH are persistent, bioaccumulate in the environment, and are detected in human breast milk and adipose tissues. DDT exposures have been previously shown to disrupt insulin signaling and glucoregulation, increasing risk for diabetes. We have previously shown that embryonic exposures organochlorines such as polychlorinated biphenyls disrupted pancreatic development and early embryonic glucoregulatory networks. Here, we determined the impacts of the similar compounds TCPM and TCPMOH on zebrafish pancreatic growth and gene expression following developmental exposures.
Methods
Zebrafish embryos were exposed to 50 nM TCPM or TCPMOH beginning at 24 hr postfertilization (hpf) and exposures were refreshed daily. At 96 hpf, pancreatic growth and islet area were directly visualized in Tg(ptf1a::GFP) and Tg(insulin::GFP) embryos, respectively, using microscopy. Gene expression was assessed at 100 hpf with RNA sequencing.
Results
Islet and total pancreas area were reduced by 20.8% and 13% in embryos exposed to 50 nM TCPMOH compared to controls. TCPM did not induce significant morphological changes to the developing pancreas, indicating TCPMOH, but not TCPM, impairs pancreatic development despite similarity in molecular responses. Transcriptomic responses to TCPM and TCPMOH were correlated (R2 = .903), and pathway analysis found downregulation of processes including retinol metabolism, circadian rhythm, and steroid biosynthesis.
Conclusion
Overall, our data suggest that TCPM and TCPMOH may be hazardous to embryonic growth and development.
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