Background

Exposure assessment is critical for connecting environmental pollutants to health outcomes and evaluating impacts of interventions or environmental policies. Silicone wristbands (SWBs) show promise for multi-pollutant exposure assessment, including polycyclic aromatic hydrocarbons (PAHs), a ubiquitous class of toxic environmental pollutants.

Objective

To review published studies where SWBs were worn on the wrist for human environmental exposure assessments and evaluate the ability of SWBs to capture personal exposures, identify gaps which need to be addressed to implement this tool, and make recommendations for future studies to advance the field of exposure science through utilization of SWBs.

Methods

We performed a systematic search and a cited reference search in Scopus and extracted key study descriptions.

Results

Thirty-nine unique studies were identified, with analytes including PAHs, pesticides, flame retardants, and tobacco products. SWBs were shipped under ambient conditions without apparent analyte loss, indicating utility for global exposure and health studies. Nineteen articles detected a total of 60 PAHs in at least one SWB. Correlations with other concurrent biological and air measurements indicate the SWB captures exposure to flame retardants, tobacco products, and PAHs.

Significance

SWBs show promise as a simple-to-deploy tool to estimate environmental and occupational exposures to chemical mixtures, including PAHs.

This cross-sectional study examines the prevalence of and income-related disparities associated with exposure to thirdhand smoke among children.

Introduction

Environmental exposure to lead (Pb) and cadmium (Cd) are risk factors for adverse health outcomes in children and adults. This study examined whether thirdhand smoke residue contributes to Pb and Cd in settled house dust.

Methods

Participants were 60 multiunit housing residents in San Diego, California. All had indoor smoking bans during the study period, and 55 were nonsmokers. Wipe samples from different surfaces and vacuum floor dust samples were analyzed for nicotine, a marker of thirdhand smoke, and for Pb and Cd using liquid chromatography-triple quadrupole mass spectrometry and inductively coupled plasma-mass spectrometry, respectively.

Results

Examined in each sample type separately, Pb and Cd loadings were significantly correlated (r = 0.73, vacuum floor dust; 0.52, floor wipes; 0.72, window sill/trough wipes; all p < 0.0025). Pb and Cd loadings from different sample types were not correlated (all p > 0.30). Nicotine loading in dust was significantly correlated with Pb and Cd loading in dust (r = 0.49 for Pb; r = 0.39 for Cd, all p < 0.0025). Pb and Cd loadings on floor or window surfaces, showed no association with nicotine loading in dust, on floors, or on furniture (all p < 0.30).

Conclusions

Tobacco smoke is a likely source of Pb and Cd that accumulates in settled house dust in multiunit housing, suggesting that Pb and Cd are constituents of thirdhand smoke that lingers long after smoking has ended.

Secondhand smoke (SHS) exposure is a major cause of illnesses in children and leaves a persistent and toxic residue indoors called thirdhand smoke (THS) that adheres to various surfaces, permeates materials, accumulates in household dust, and is subsequently re-emitted into the air. THS, like SHS, has been shown to contain multiple toxic chemicals, including carcinogenic tobacco-specific nitrosamines (TSNAs). Children are highly susceptible to tobacco smoke pollutants, and simple methods for assessing children’s SHS and THS exposure are needed. Therefore, we evaluated the performance of a cotton pillow used as a passive sampler in homes of children with caregivers who smoke tobacco, with and without home smoking bans, as well as nonsmokers. We deployed a commercially available organic cotton travel pillow, which was left in the home for a median of 9.1 days. Pillow component nicotine levels were significantly higher in homes of smokers without a ban as compared to smokers and nonsmokers who had a ban (e.g., median pillowcase nicotine 337.7 ng/g per day vs. 72.5 ng/g per day and 0.1 ng/g per day, respectively) and differences were similar to those for air nicotine. Pillowcase TSNAs were detected mainly in the homes of smokers without a smoking ban. Pillow component (pillowcase, fabric, and filling) nicotine levels were highly correlated with air nicotine levels (rho = 0.76-0.88, all P < 0.001). Nicotine in the pillow components was also highly correlated with urinary cotinine in the children (rho = 0.65 to 0.81, all P < 0.001) and other measures of tobacco smoke exposure. Pillow performance as a sampler is promising, given the ease and simplicity of sample deployment.

Cigarette butts are one of the most prevalent forms of litter worldwide and may leach toxic compounds when deposited in aquatic environments. Previous studies demonstrated that smoked cigarette leachate is toxic toward aquatic organisms. However, the specific bioavailable chemicals from the leachate and the potential for human and wildlife exposure through the food chain were unknown. Using a nontargeted analytical approach based on GC×GC/TOF-MS, 43 compounds were confirmed to leach from smoked cigarettes when exposed to a water source. Additionally, the bioaccumulation potential of organic contaminants in an edible fish, rainbow trout (Oncorhynchus mykiss), was assessed through direct exposure to the leachate of smoked cigarettes at 0.5 CB/L for 28 days. There was a significant reduction in fish mass among the exposed rainbow trout vs the control group (χ² (1) = 5.3, p = 0.021). Both nontargeted and targeted chemical analysis of representative fish tissue identified four tobacco alkaloids, nicotine, nicotyrine, myosmine, and 2,2'-bipyridine. Their average tissue concentrations were 466, 55.4, 94.1, and 70.8 ng/g, respectively. This study identifies leached compounds from smoked cigarettes and demonstrates the uptake of specific chemicals in rainbow trout, thus suggesting a potential for accumulation in food webs, resulting in human and wildlife exposure.

Thirdhand smoke (THS) is the persistent and toxic residue from tobacco smoke in indoor environments. A comprehensive understanding of the chemical constituents of THS is necessary to assess the risks of long-term exposure and to establish reliable THS tracers. The objective of this study was to investigate compounds associated with THS through nontargeted analysis (NTA) of settled house dust samples from smokers' and non-smokers' homes, using comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC×GC/TOF-MS). Compounds that were either only present in dust from smokers' homes or that had significantly larger abundance than in non-smokers' homes were termed qualified compounds. We identified 140 qualified compounds, and of these, 42 compounds were tentatively identified by searching matching mass spectra in NIST electron impact (EI) mass spectral library including 20 compounds confirmed with their authentic standards. Among the 42 compounds, 26 compounds were statistically more abundant (p < 0.10) in dust from homes of smokers; seven were tobacco-specific compounds, two of which (nornicotyrine, 3-ethenylpyridine) have not been reported before in house dust. Two compounds, tris (2-chloroethyl) phosphate (a toxic compound used as a flame retardant and reported in tobacco) and propanoic acid, 2-methyl-, 1-(1,1-dimethylethyl)-2-methyl-1,3-propanediyl ester (highly abundant and reported in exhaled air of smokers), were found in dust from all smokers' homes and in zero non-smokers' homes, making these potential THS tracers, possibly associated with recent smoking. Benzyl methyl ketone was significantly higher in dust in smokers' homes, and was previously reported not as a product of tobacco but rather as a form of methamphetamine. This compound was recently reported in mainstream tobacco smoke condensate through NTA as well. These identified potential tracers and chemical components of THS in this study can be further investigated for use in developing THS contamination and exposure assessments.

Understanding the health implications of human exposure to mixtures of chemical contaminants is aided by analytical methods that can screen for a broad range of both expected and unexpected compounds. We performed a proof-of-concept analysis combining human breast milk, a biomonitoring matrix for determining contaminant exposure to mothers and infants, with a non-targeted method based on comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC×GC/TOF-MS). A total of 172 presumably anthropogenic halogenated compounds and non-halogenated cyclic and aromatic compounds were tentatively identified in breast milk from San Diego, California through mass spectral database searches. Forty of the compounds were prioritized for confirmation based on halogenation or 100% frequency of detection, and the identities of 30 were verified using authentic standards. Thirty-four (85%) of the prioritized contaminants are not typically monitored in breast milk surveys, and 31 (77%) are regulated in at least one market worldwide, indicating breast milk may be a useful biomonitoring matrix for non-targeted analysis and the assessment of human exposure to future emerging or undiscovered contaminants.

Exposure assessment in children, especially young children, presents difficulties not found with adults. Simple silicone wristbands are passive samplers that have potential applicability in exposure studies of children. We investigated the performance of silicone wristbands as personal nicotine samplers in two wristbands worn by a child (n = 31) for 7 days and for 2 days (worn day 5 to day 7). We compared levels of nicotine in wristbands with urinary cotinine, a metabolite of nicotine, measured in the child's urine obtained on day 7. Children were recruited who were exposed to contaminants in tobacco smoke and/or vapor from electronic nicotine delivery systems (ENDS; commonly known as electronic cigarettes or EC) as well as children who lived in nonsmoking homes. Caregivers were interviewed to obtain reported measures of the child's exposure. Analysis was by liquid chromatography with triple quadrupole mass spectrometry and isotope dilution (LC-MS/MS). The nicotine detected in the wristbands worn for 2 days was highly correlated with urinary cotinine concentration (df = 29, r² = 0.741, p < 0.001), as was nicotine in wristbands worn for 7 days (df = 28, r² = 0.804, p < 0.001). The 2- and 7-day wristband nicotine amounts were also significantly correlated (df = 28, r² = 0.852, p < 0.001). Silicone wristbands may be a useful tool for epidemiological and intervention studies of tobacco product exposure in children.

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 library of halogenated organic compounds (HOCs) consisted of 180 anthropogenic contaminants, 41 natural products, 4 with mixed sources, 8 with unknown sources, and 94 with partial structural characterization and unknown sources. The abundance of compounds whose structures could not be fully elucidated highlights the prevalence of undiscovered HOCs accumulating in marine food webs. Eighty-six percent of the identified compounds are not currently monitored, including 133 known anthropogenic chemicals. Compounds related to dichlorodiphenyltrichloroethane (DDT) were the most abundant. Natural products were, in some cases, detected at abundances similar to anthropogenic compounds. The profile of naturally occurring HOCs differed between ecotypes, suggesting more abundant offshore sources of these compounds. This nontargeted analytical framework provided a comprehensive list of HOCs that may be characteristic of the region, and its application within monitoring surveys may suggest new chemicals for evaluation.