High-Resolution Mass Spectrometry for Human Exposomics: Expanding Chemical Space Coverage.

In the modern "omics" era, measurement of the human exposome is a critical missing link between genetic drivers and disease outcomes. High-resolution mass spectrometry (HRMS), routinely used in proteomics and metabolomics, has emerged as a leading technology to broadly profile chemical exposure agents and related biomolecules for accurate mass measurement, high sensitivity, rapid data acquisition, and increased resolution of chemical space. Non-targeted approaches are increasingly accessible, supporting a shift from conventional hypothesis-driven, quantitation-centric targeted analyses toward data-driven, hypothesis-generating chemical exposome-wide profiling. However, HRMS-based exposomics encounters unique challenges. New analytical and computational infrastructures are needed to expand the analysis coverage through streamlined, scalable, and harmonized workflows and data pipelines that permit longitudinal chemical exposome tracking, retrospective validation, and multi-omics integration for meaningful health-oriented inferences. In this article, we survey the literature on state-of-the-art HRMS-based technologies, review current analytical workflows and informatic pipelines, and provide an up-to-date reference on exposomic approaches for chemists, toxicologists, epidemiologists, care providers, and stakeholders in health sciences and medicine. We propose efforts to benchmark fit-for-purpose platforms for expanding coverage of chemical space, including gas/liquid chromatography-HRMS (GC-HRMS and LC-HRMS), and discuss opportunities, challenges, and strategies to advance the burgeoning field of the exposome.

Association between Personal Abiotic Airborne Exposures and Body Composition Changes among Healthy Adults (60-69 Years Old): A Combined Exposome-Wide and Lipidome Mediation Approach from the China BAPE Study.

BACKGROUND: Evidence suggested that abiotic airborne exposures may be associated with changes in body composition. However, more evidence is needed to identify key pollutants linked to adverse health effects and their underlying biomolecular mechanisms, particularly in sensitive older adults. OBJECTIVES: Our research aimed to systematically assess the relationship between abiotic airborne exposures and changes in body composition among healthy older adults, as well as the potential mediating mechanisms through the serum lipidome. METHODS: From September 2018 to January 2019, we conducted a monthly survey among 76 healthy adults (60-69 years old) in the China Biomarkers of Air Pollutant Exposure (BAPE) study, measuring their personal exposures to 632 abiotic airborne pollutions using MicroPEM and the Fresh Air wristband, 18 body composition indicators from the InBody 770 device, and lipidomics from venous blood samples. We used an exposome-wide association study (ExWAS) and deletion/substitution/addition (DSA) model to unravel complex associations between exposure to contaminant mixtures and body composition, a Bayesian kernel machine regression (BKMR) model to assess the overall effect of key exposures on body composition, and mediation analysis to identify lipid intermediators. RESULTS: The ExWAS and DSA model identified that 2,4,5-T methyl ester (2,4,5-TME), 9,10-Anthracenedione (ATQ), 4b,8-dimethyl-2-isopropylphenanthrene, and 4b,5,6,7,8,8a,9,10-octahydro-(DMIP) were associated with increased body fat mass (BFM), fat mass indicators (FMI), percent body fat (PBF), and visceral fat area (VFA) in healthy older adults [Bonferroni-Hochberg false discovery rate (FDRBH)<0.05]. The BKMR model demonstrated a positive correlation between contaminants (anthracene, ATQ, copaene, di-epi-α-cedrene, and DMIP) with VFA. Mediation analysis revealed that phosphatidylcholine [PC, PC(16:1e/18:1), PC(16:2e/18:0)] and sphingolipid [SM, SM(d18:2/24:1)] mediated a significant portion, ranging from 12.27% to 26.03% (p-value <0.05), of the observed increase in VFA. DISCUSSION: Based on the evidence from multiple model results, ATQ and DMIP were statistically significantly associated with the increased VFA levels of healthy older adults, potentially regulated through lipid intermediators. These findings may have important implications for identifying potentially harmful environmental chemicals and developing targeted strategies for the control and prevention of chronic diseases in the future, particularly as the global population is rapidly aging. https://doi.org/10.1289/EHP13865.

Personal exposure to airborne organic pollutants and lung function changes among healthy older adults.

Epidemiological evidence on the impact of airborne organic pollutants on lung function among the elderly is limited, and their underlying biological mechanisms remain largely unexplored. Herein, a longitudinal panel study was conducted in Jinan, Shandong Province, China, involving 76 healthy older adults monitored over a span of five months repetitively. We systematically evaluated personal exposure to a diverse range of airborne organic pollutants using a wearable passive sampler and their effects on lung function. Participants' pulmonary function indicators were assessed, complemented by comprehensive multi-omics analyses of blood and urine samples. Leveraging the power of interaction analysis, causal inference test (CIT), and integrative pathway analysis (IPA), we explored intricate relationships between specific organic pollutants, biomolecules, and lung function deterioration, elucidating the biological mechanisms underpinning the adverse impacts of these pollutants. We observed that bis (2-chloro-1-methylethyl) ether (BCIE) was significantly associated with negative changes in the forced vital capacity (FVC), with glycerolipids mitigating this adverse effect. Additionally, 31 canonical pathways [e.g., high mobility group box 1 (HMGB1) signaling, phosphatidylinositol 3-kinase (PI3K)/AKT pathway, epithelial mesenchymal transition, and heme and nicotinamide adenine dinucleotide (NAD) biosynthesis] were identified as potential mechanisms. These findings may hold significant implications for developing effective strategies to prevent and mitigate respiratory health risks arising from exposure to such airborne pollutants. However, due to certain limitations of the study, our results should be interpreted with caution.

Behavioral skills training for teaching safety skills to mental health service providers compared to training-as-usual: a pragmatic randomized control trial.

BACKGROUND: Violence in the healthcare workplace has been a global concern for over two decades, with a high prevalence of violence towards healthcare workers reported. Workplace violence has become a healthcare quality indicator and embedded in quality improvement initiatives of many healthcare organizations. The Centre for Addiction and Mental Health (CAMH), Canada's largest mental health hospital, provides all clinical staff with mandated staff safety training for self-protection and team-control skills. These skills are to be used as a last resort when a patient is at imminent risk of harm to self or others. The purpose of this study is to compare the effectiveness of two training methods of this mandated staff safety training for workplace violence in a large psychiatric hospital setting. METHODS: Using a pragmatic randomized control trial design, this study compares two approaches to teaching safety skills CAMH's training-as-usual (TAU) using the 3D approach (description, demonstration and doing) and behavioural skills training (BST), from the field of applied behaviour analysis, using instruction, modeling, practice and feedback loop. Staff were assessed on three outcome measures (competency, mastery and confidence), across three time points: before training (baseline), immediately after training (post-training) and one month later (follow-up). This study was registered with the ISRCTN registry on 06/09/2023 (ISRCTN18133140). RESULTS: With a sample size of 99 new staff, results indicate that BST was significantly better than TAU in improving observed performance of self-protection and team-control skills. Both methods were associated with improved skills and confidence. However, there was a decrease in skill performance levels at the one-month follow-up for both methods, with BST remaining higher than TAU scores across all three time points. The impact of training improved staff confidence in both training methods and remained high across all three time points. CONCLUSIONS: The study findings suggest that BST is more effective than TAU in improving safety skills among healthcare workers. However, the retention of skills over time remains a concern, and therefore a single training session without on-the-job-feedback or booster sessions based on objective assessments of skill may not be sufficient. Further research is needed to confirm and expand upon these findings in different settings.

Using unsupervised clustering approaches to identify common mental health profiles and associated mental health-care service-use patterns in Ontario, Canada.

Mental health is a complex, multidimensional concept that goes beyond clinical diagnoses, including psychological distress, life stress, and well-being. In this study, we aimed to use unsupervised clustering approaches to identify multidimensional mental health profiles that exist in the population, and their associated service-use patterns. The data source was the 2012 Canadian Community Health Survey-Mental Health, linked to administrative health-care data; all Ontario, Canada, adult respondents were included. We used a partitioning around medoids clustering algorithm with Gower's proximity to identify groups with distinct combinations of mental health indicators and described them according to their sociodemographic and service-use characteristics. We identified 4 groups with distinct mental health profiles, including 1 group that met the clinical threshold for a depressive diagnosis, with the remaining 3 groups expressing differences in positive mental health, life stress, and self-rated mental health. The 4 groups had different age, employment, and income profiles and exhibited differential access to mental health-care services. This study represents the first step in identifying complex profiles of mental health at the population level in Ontario. Further research is required to better understand the potential causes and consequences of belonging to each of the mental health profiles identified. This article is part of a Special Collection on Mental Health.

A balancing act: navigating the nuances of co-production in mental health research.

BACKGROUND: In the context of mental health research, co-production involves people with lived expertise, those with professional or academic expertise, and people with both of these perspectives collaborating to design and actualize research initiatives. In the literature, two dominant perspectives on co-production emerge. The first is in support of co-production, pointing to the transformative value of co-production for those involved, the quality of services developed through this process, as well as to broader system-level impacts (e.g. influencing changes in health system decision making, care practices, government policies, etc.). The second stance expresses scepticism about the capacity of co-production to engender genuine collaboration given the deeply ingrained power imbalances in the systems in which we operate. While some scholars have explored the intersections of these two perspectives, this body of literature remains limited. MAIN TEXT: This paper contributes to the literature base by exploring the nuances of co-production in health research. Using our mental health participatory action research project as a case example, we explore the nuances of co-production through four key values that we embraced: 1. Navigating power relations together 2. Multi-directional learning 3. Slow and steady wins the race 4. Connecting through vulnerability CONCLUSIONS: By sharing these values and associated principles and practices, we invite readers to consider the complexities of co-production and explore how our experiences may inform their practice of co-production. Despite the inherent complexity of co-production, we contend that pursuing authentic and equitable collaborations is integral to shaping a more just and inclusive future in mental health research and the mental health system at large.

BACKGROUND: In the context of mental health research, co-production is a process where people with lived experiences, those with academic or professional experience, and people with both of these perspectives collaborate to design and actualize research initiatives. In the literature, there are two main opinions about co-production. The first opinion is that co-production is beneficial for those involved, improves the quality of services, and can also have impacts at higher system levels (e.g. influencing changes in health system decision making, care practices, government policies, etc.). The second opinion is doubtful that co-production has the ability to foster authentic collaboration because of the differences in power between academic and health systems. Even though some scholars have looked at both opinions, there is not a lot of research on this. MAIN TEXT: This paper contributes to the literature base exploring the nuances of co-production in health research. Using our mental health participatory action research project as a case example, we explore the nuances of co-production through four key values that we embraced: 1. Navigating power relations together 2. Multi-directional learning 3. Slow and steady wins the race 4. Connecting through vulnerability CONCLUSIONS: By sharing these values and associated principles and practices, we invite readers to consider the complexities of co-production and explore how our process may inform their engagement with co-production. We argue that pursuing authentic collaborations is key to shaping a more just and inclusive future in mental health research and the mental health system at large.

PolyMatch: Novel Libraries, Algorithms, and Visualizations for Discovering Polymers and Chemical Series.

Polymers are integral components of everyday products, ranging from plastics and emulsifiers to lubricants and detergents. Characterization of these materials at the molecular level is essential to understanding their physicochemical properties and potential health impacts, considering factors such as the number of repeating units, chemical moieties, functional groups, and degree of unsaturation. This study introduces a free open-source vendor neutral software, PolyMatch, designed to annotate polysorbates, polysorbides, polyethylene glycols (PEGs), fatty acid esterified species, and related chemical species based on mass spectral and chromatographic patterns inherent in the repeating nature of chemical moieties. PolyMatch facilitates the generation of MS/MS libraries for polymeric chemical species characterization (with over 800 000 structures with associated fragment masses already built in) and covers the entire liquid chromatography-high-resolution mass spectrometry (LC-HRMS/MS) data-processing workflow. PolyMatch covers peak picking, blank filtering, annotation, data visualization, and sharing of interactive data sets via an HTML link to the community. The software was applied to a Tween 80 mixture, using LC-HRMS/MS on an Agilent 6546 Q-TOF instrument with iterative exclusion for comprehensive fragmentation coverage. PolyMatch automatically assigned 86 features with high confidence at the species level, 362 based on PEG containing fragments and accurate mass matching to a simulated polymer database, and over 10 000 based on being a member of a homologous series (three or more) with CH2CH2O repeating units. The ease of use of PolyMatch and comprehensive coverage with species level assignment is expected to contribute to the advancement of materials science, health research, and product development.

Intellectual and developmental disabilities in Ontario's criminal justice and forensic mental health systems: Using data to tell the story.

BACKGROUND: International studies show that adults with intellectual and developmental disabilities (IDD) are disproportionately represented in the criminal justice and forensic mental health systems; however, it is difficult to capture their involvement across systems in any one jurisdiction. AIMS: The current study aimed to estimate the prevalence of IDD across different parts of the criminal justice and forensic mental health systems in Ontario and to describe the demographic and clinical profiles of these individuals relative to their counterparts without IDD. METHODS: This project utilised administrative data to identify and describe the demographic and clinical characteristics of adults with IDD and criminal justice or forensic involvement across four sectors: federal correctional facilities, provincial correctional facilities, forensic inpatient mental health care and community mental health programmes. Questions were driven by and results were contextualised by a project advisory group and people with lived experience from the different sectors studied, resulting in a series of recommendations. RESULTS: Adults with IDD were over-represented in each of the four settings, ranging from 2.1% in federal corrections to 16.7% in forensic inpatient care. Between 20% (forensic inpatient) and 38.4% (provincial corrections) were under the age of 25 and between 34.5% (forensic inpatient) and 41.8% (provincial corrections) resided in the lowest income neighbourhoods. Medical complexity and rates of co-occurring mental health conditions were higher for people with IDD than those without IDD in federal and provincial corrections. CONCLUSIONS: Establishing a population-based understanding of people with IDD within these sectors is an essential first step towards understanding and addressing service and care needs. Building on the perspectives of people who work in and use these systems, this paper concludes with intervention recommendations before, during and after justice involvement.

Assessment of wood smoke induced pulmonary toxicity in normal- and chronic bronchitis-like bronchial and alveolar lung mucosa models at air-liquid interface.

BACKGROUND: Chronic obstructive pulmonary disease (COPD) has the highest increased risk due to household air pollution arising from biomass fuel burning. However, knowledge on COPD patho-mechanisms is mainly limited to tobacco smoke exposure. In this study, a repeated direct wood smoke (WS) exposure was performed using normal- (bro-ALI) and chronic bronchitis-like bronchial (bro-ALI-CB), and alveolar (alv-ALI) lung mucosa models at air-liquid interface (ALI) to assess broad toxicological end points. METHODS: The bro-ALI and bro-ALI-CB models were developed using human primary bronchial epithelial cells and the alv-ALI model was developed using a representative type-II pneumocyte cell line. The lung models were exposed to WS (10 min/exposure; 5-exposures over 3-days; n = 6-7 independent experiments). Sham exposed samples served as control. WS composition was analyzed following passive sampling. Cytotoxicity, total cellular reactive oxygen species (ROS) and stress responsive NFkB were assessed by flow cytometry. WS exposure induced changes in gene expression were evaluated by RNA-seq (p ≤ 0.01) followed by pathway enrichment analysis. Secreted levels of proinflammatory cytokines were assessed in the basal media. Non-parametric statistical analysis was performed. RESULTS: 147 unique compounds were annotated in WS of which 42 compounds have inhalation toxicity (9 very high). WS exposure resulted in significantly increased ROS in bro-ALI (11.2%) and bro-ALI-CB (25.7%) along with correspondingly increased NFkB levels (bro-ALI: 35.6%; bro-ALI-CB: 18.1%). A total of 1262 (817-up and 445-down), 329 (141-up and 188-down), and 102 (33-up and 69-down) genes were differentially regulated in the WS-exposed bro-ALI, bro-ALI-CB, and alv-ALI models respectively. The enriched pathways included the terms acute phase response, mitochondrial dysfunction, inflammation, oxidative stress, NFkB, ROS, xenobiotic metabolism of AHR, and chronic respiratory disorder. The enrichment of the 'cilium' related genes was predominant in the WS-exposed bro-ALI (180-up and 7-down). The pathways primary ciliary dyskinesia, ciliopathy, and ciliary movement were enriched in both WS-exposed bro-ALI and bro-ALI-CB. Interleukin-6 and tumor necrosis factor-α were reduced (p < 0.05) in WS-exposed bro-ALI and bro-ALI-CB. CONCLUSION: Findings of this study indicate differential response to WS-exposure in different lung regions and in chronic bronchitis, a condition commonly associated with COPD. Further, the data suggests ciliopathy as a candidate pathway in relation to WS-exposure.

Understanding Quality Improvement and Continuing Professional Mentorship: A Needs Assessment Study to Inform the Development of a Community of Practice.

INTRODUCTION: Quality improvement (QI) programming attempts to bridge the gap between patient care and standards of care. Mentorship could be a means through which QI is fostered, developed, and incorporated into continuing professional development (CPD) programs. The current study examined (1) models of implementation for mentorship within the Department of Psychiatry of a large Canadian academic center; (2) mentorship as a potential vehicle for alignment of QI practices and CPD; and (3) needs for the implementation of QI and CPD mentorship programs. METHODS: Qualitative interviews were conducted with 14 individuals associated with the university's Department of Psychiatry. The data were analyzed through thematic analyses with two independent coders using COREQ guidelines. RESULTS: Our results identified uncertainty among the participants regarding the conceptualization of QI and CPD, illustrating difficulties in determining whether mentorship could be used to align these practices. Three major themes were identified in our analyses: sharing of QI work through communities of practices; the need for organizational support; and relational experiences of QI mentoring. DISCUSSION: A greater understanding of QI is necessary before psychiatry departments can implement mentorship to enhance QI practices. However, models of mentorship and needs for mentorship have been made clear and include a good mentorship fit, organizational support, and opportunities for both formal and informal mentorship. Changing organizational culture and providing appropriate training is necessary for enhancing QI.

Finding connection "while everything is going to crap": experiences in Recovery Colleges during the COVID-19 pandemic.

BACKGROUND: Recovery Colleges (RCs) are mental health and well-being education centres where people come together and learn skills that support their wellness. Co-production, co-learning and transformative education are fundamental to RCs. People with lived experience are recognized as experts who partner with health professionals in the design and actualization of educational programming. The pandemic has changed how RCs operate by necessitating a shift from in-person to virtual offerings. Given the relational ethos of RCs, it is important to explore how the experiences of RC members and communities were impacted during this time. To date, there has been limited scholarship on this topic. METHODS: In this exploratory phase of a larger project, we used participatory action research to interview people who were accessing, volunteering and/or working in RCs across Canada. Semi-structured interviews were conducted with twenty-nine individuals who provided insights on what is important to them about RC programming. RESULTS: Our study was conducted amid the COVID-19 pandemic. Accordingly, participants elucidated how their involvement in RCs was impacted by pandemic related restrictions. The results of this study demonstrate that RC programming is most effective when it: (1) is inclusive; (2) has a "good vibe"; and (3) equips people to live a fuller life. CONCLUSIONS: The pandemic, despite its challenges, has yielded insights into a possible evolution of the RC model that transcends the pandemic-context. In a time of great uncertainty, RCs served as safe spaces where people could redefine, pursue, maintain or recover wellness on their own terms.

BACKGROUND: Recovery Colleges (RCs) are mental health and well-being education centres where people come together and learn skills that support their personal recovery journeys. WHAT DID WE WANT TO KNOW? WHAT APPROACH DID WE TAKE?: In this phase of a larger project, we used a participatory action research approach to interview people who were accessing, volunteering and/or working in RCs across Canada. This research approach draws on the knowledge of all researchers and participants and places equal value on personal and professional experiences. Therefore, this study was created and shaped by, with, and for people who participate in RCs in partnership with academic researchers. WHAT DID WE DO?: Twenty-nine individuals shared what is important to them about RC programming. Our study took place during the COVID-19 pandemic during the pandemic-related restrictions such as social distancing. WHAT DID WE LEARN?: The results of this study demonstrate that RC programming is most effective when it: (1) is inclusive; (2) has a "good vibe"; and (3) equips people to live a fuller life. The pandemic, despite its challenges, could inform an evolution of the RC model that lasts beyond the pandemic.

Per- and polyfluoroalkyl substances (PFAS) and thyroid hormone measurements in dried blood spots and neonatal characteristics: a pilot study.

BACKGROUND: Pediatric thyroid diseases have been increasing in recent years. Environmental risk factors such as exposures to chemical contaminants may play a role but are largely unexplored. Archived neonatal dried blood spots (DBS) offer an innovative approach to investigate environmental exposures and effects. OBJECTIVE: In this pilot study, we applied a new method for quantifying per- and polyfluoroalkyl substances (PFAS) to 18 archived DBS from babies born in California from 1985-2018 and acquired thyroid hormone measurements from newborn screening tests. Leveraging these novel data, we evaluated (1) changes in the concentrations of eight PFAS over time and (2) the relationship between PFAS concentrations, thyroid hormone concentrations, and neonatal characteristics to inform future research. METHODS: PFAS concentrations in DBS were measured using ultra-high-performance liquid chromatography-mass spectrometry. Summary statistics and non-parametric Wilcoxon rank-sum and Kruskal-Wallis tests were used to evaluate temporal changes in PFAS concentrations and relationships between PFAS concentrations, thyroid hormone concentrations, and neonatal characteristics. RESULTS: The concentration and detection frequencies of several PFAS (PFOA, PFOS, and PFOSA) declined over the assessment period. We observed that the timing of specimen collection in hours after birth was related to thyroid hormone but not PFAS concentrations, and that thyroid hormones were related to some PFAS concentrations (PFOA and PFOS). IMPACT STATEMENT: This pilot study examines the relationship between concentrations of eight per- and polyfluoroalkyl substances (PFAS), thyroid hormone levels, and neonatal characteristics in newborn dried blood spots (DBS) collected over a period of 33 years. To our knowledge, 6 of the 22 PFAS we attempted to measure have not been quantified previously in neonatal DBS, and this is the first study to examine both PFAS and thyroid hormone concentrations using DBS. This research demonstrates the feasibility of using newborn DBS for quantifying PFAS exposures in population-based studies, highlights methodological considerations in the use of thyroid hormone data for future studies using newborn DBS, and indicates potential relationships between PFAS concentrations and thyroid hormones for follow-up in future research.

Aquatic Vegetation, an Understudied Depot for PFAS.

Per- and polyfluoroalkyl substances (PFAS) are a class of manufactured chemicals that have been extensively utilized worldwide. We hypothesize that the presence, uptake, and accumulation of PFAS in aquatic vegetation (AV) is dependent upon several factors, such as the physiochemical properties of PFAS and proximity to potential sources. In this study, AV was collected from eight locations in Florida to investigate the PFAS presence, accumulation, and spatiotemporal distribution. PFAS were detected in AV at all sampling locations, with a range from 0.18 to 55 ng/g sum (∑)PFAS. Individual PFAS and their concentrations varied by sampling location, time, and AV species. A total of 12 PFAS were identified, with the greatest concentrations measured in macroalgae. The average bioconcentration factor (BCF) among all samples was 1225, indicating high PFAS accumulation in AV from surface water. The highest concentrations, across all AV types, were recorded in the Indian River Lagoon (IRL), a location with a history of elevated PFAS burdens. The present study represents the first investigation of PFAS in naturally existing estuarine AV, filling an important gap on PFAS partitioning within the environment, as well as providing insights into exposure pathways for aquatic herbivores. Examining the presence, fate, and transport of these persistent chemicals in Florida's waterways is critical for understanding their effect on environmental, wildlife, and human health.

Adequacy of stationary measurements as proxies for residential personal exposure to gaseous and particle air pollutants.

People are exposed to myriad of airborne pollutants in their homes. Owing to diverse potential sources of air pollution and human activity patterns, accurate assessment of residential exposures is complex. In this study, we explored the relationship between personal and stationary air pollutant measurements in residences of 37 participants working from home during the heating season. Stationary environmental monitors (SEMs) were located in the bedroom, living room or home office and personal exposure monitors (PEMs) were worn by the participants. SEMs and PEMs included both real-time sensors and passive samplers. During three consecutive weekdays, continuous data were obtained for particle number concentration (size range 0.3-10 µm), carbon dioxide (CO2), and total volatile organic compounds (TVOC), while passive samplers collected integrated measures of 36 volatile organic compounds (VOCs) and semi volatile organic compounds (SVOCs). The personal cloud effect was detected in >80% of the participants for CO2 and >50% participants for PM10. Multiple linear regression analysis showed that a single CO2 monitor placed in the bedroom efficiently represented personal exposure to CO2 (R2 = 0.90) and moderately so for PM10 (R2 = 0.55). Adding a second or third sensor in a residence did not lead to improved exposure estimates for CO2, with only 6-9% improvement for particles. Selecting data from SEMs when participants were in the same room improved personal exposure estimates by 33% for CO2 and 5% for particles. Out of 36 detected VOCs and SVOCs, 13 had at least 50% higher concentrations in personal versus stationary samples. Findings from this study aid improved understanding of the complex dynamics of gaseous and particle pollutants and their sources in residences, and could support the development of refined procedures for residential air quality monitoring and inhalation exposure assessment.

Trace analysis of per- and polyfluorinated alkyl substances (PFAS) in dried blood spots - Demonstration of reproducibility and comparability to venous blood samples.

Per- and polyfluoroalkyl substances (PFAS) are a group of man-made chemicals that have been widely used in consumer, personal care, and household products for their stain- and water-repellent properties. PFAS exposure has been linked to various adverse health outcomes. Such exposure has commonly been evaluated in venous blood samples. While this sample type can be obtained from healthy adults, a less invasive method of blood collection is required when evaluating vulnerable populations. Dried blood spots (DBS) have gained attention as a biomatrix for exposure assessment given the relative ease of collection, transport, and storage. The objective of this study was to develop and validate an analytical method to measure PFAS in DBS. A workflow is presented for extracting PFAS from DBS, chemical analysis by liquid chromatography-high resolution mass spectrometry, normalization for blood mass, and blank correction to account for potential contamination. Over 80 % recovery was achieved for the 22 PFAS measured with an average coefficient of variation of 14 %. Comparison of PFAS concentrations detected in DBS and paired whole blood samples from six healthy adults was correlated (R2 > 0.9). Findings demonstrate trace levels of a broad range of PFAS in DBS can be reproducibly measured and are comparable to liquid whole blood samples. DBS can offer novel insights to environmental exposures, including during critical windows of susceptibility (i.e., in utero, early life), which have been largely uncharacterized.

Novel perfluoroalkyl substances (PFAS) discovered in whole blood using automated non-targeted analysis of dried blood spots.

A small subset of per- and polyfluoroalkyl substances (PFAS) are routinely screened in human blood. These compounds generally explain <50 % of the total PFAS in human blood. The percentage of known PFAS in human blood has been decreasing as replacement PFAS and more complex PFAS chemistries are introduced to the market. Most of these novel PFAS have not been previously identified. Non-targeted methods are required to characterize this "dark matter" PFAS. Our objective was to apply non-targeted PFAS analysis to human blood to gain an understanding about the sources, concentrations, and toxicity of these compounds. A high-resolution tandem mass spectrometry (HRMS) and software workflow for PFAS characterization in dried blood spots is reported. Dried blood spots are a less invasive collection technique compared to venous blood draws, allowing collection from vulnerable populations. Biorepositories of archived dried blood spots are available internationally from newborns and present opportunities to study prenatal exposure to PFAS. In this study, dried blood spot cards were analyzed using iterative MS/MS by liquid chromatography HRMS. Data processing was conducted using FluoroMatch Suite including a visualizer tool that presents homologous series, retention time vs m/z plots, MS/MS spectra, feature tables, annotations, and fragments for fragment screening. The researcher performing data-processing and annotation was blinded to the fact that standards were spiked in, and was able to annotate 95 % of standards spiked on dried blood spot samples, signifying a low false negative rate using FluoroMatch Suite. A total of 28 PFAS (20 standards and 4 exogenous compounds) were detected across five homologous series with Schymanski Level 2 confidence. Of these 4, 3 were perfluoroalkyl ether carboxylic acids (PFECA), a chemical class of PFAS which is increasingly being detected in environmental and biological matrices but is not currently screened in most targeted analysese. A further 86 potential PFAS were detected using fragment screening. PFAS are extremely persistent and widespread yet remain largely unregulated. Our findings will contribute to an improved an understanding of exposures. Application of these methods in environmental epidemiology studies have the potential to inform policy with regards to PFAS monitoring, regulation, and individual-level mitigation strategies.

Wearable Passive Samplers for Assessing Environmental Exposure to Organic Chemicals: Current Approaches and Future Directions.

PURPOSE OF REVIEW: We are continuously exposed to dynamic mixtures of airborne contaminants that vary by location. Understanding the compositional diversity of these complex mixtures and the levels to which we are each exposed requires comprehensive exposure assessment. This comprehensive analysis is often lacking in population-based studies due to logistic and analytical challenges associated with traditional measurement approaches involving active air sampling and chemical-by-chemical analysis. The objective of this review is to provide an overview of wearable passive samplers as alternative tools to active samplers in environmental health research. The review highlights the advances and challenges in using wearable passive samplers for assessing personal exposure to organic chemicals and further presents a framework to enable quantitative measurements of exposure and expanded use of this monitoring approach to the population scale. RECENT FINDINGS: Overall, wearable passive samplers are promising tools for assessing personal exposure to environmental contaminants, evident by the increased adoption and use of silicone-based devices in recent years. When combined with high throughput chemical analysis, these exposure assessment tools present opportunities for advancing our ability to assess personal exposures to complex mixtures. Most designs of wearable passive samplers used for assessing exposure to semi-volatile organic chemicals are currently uncalibrated, thus, are mostly used for qualitative research. The challenge with using wearable samplers for quantitative exposure assessment mostly lies with the inherent complexity in calibrating these wearable devices. Questions remain regarding how they perform under various conditions and the uncertainty of exposure estimates. As popularity of these samplers grows, it is critical to understand the uptake kinetics of chemicals and the different environmental and meteorological conditions that can introduce variability. Wearable passive samplers enable evaluation of exposure to hundreds of chemicals. The review presents the state-of-the-art of technology for assessing personal exposure to environmental chemicals. As more studies calibrate wearable samplers, these tools present promise for quantitatively assessing exposure at both the individual and population levels.

Health conditions and service use of autistic women and men: A retrospective population-based case-control study.

LAY ABSTRACT: This study used administrative data from Ontario, Canada to compare the health conditions and service use of autistic women and men with adults with other developmental disabilities and with adults without developmental disabilities. Autistic women and men were more likely to have physical and mental health conditions compared to adults without developmental disabilities. Rates of health conditions were similar or lower among autistic adults compared to adults with other developmental disabilities, except more autistic adults had psychiatric conditions. Autistic women and men used higher rates of psychiatric services compared to all other groups. When comparing autistic women with same aged autistic men, sex differences were found for specific physical (Crohn's disease/colitis, rheumatoid arthritis) and psychiatric conditions (psychotic disorders, non-psychotic disorders), as well differences in service use (emergency department visits, hospitalizations, family doctor and neurologist visits). These results further highlight the high health needs and service use of autistic women and men, as well as adults with other developmental disabilities. It is critical for future research to focus on mental health support for autistic adults and to better understand how to tailor supports to best serve autistic women.

Characterizing the external exposome using passive samplers-comparative assessment of chemical exposures using different wearable form factors.

BACKGROUND: Organic contaminants are released into the air from building materials/furnishings, personal care, and household products. Wearable passive samplers have emerged as tools to characterize personal chemical exposures. The optimal placement of these samplers on an individual to best capture airborne exposures has yet to be evaluated. OBJECTIVE: To compare personal exposure to airborne contaminants detected using wearable passive air samplers placed at different positions on the body. METHODS: Participants (n = 32) simultaneously wore four passive Fresh Air samplers, on their head, chest, wrist, and foot for 24 hours. Exposure to 56 airborne organic contaminants was evaluated using thermal desorption gas chromatography high resolution mass spectrometry with a targeted data analysis approach. RESULTS: Distinct exposure patterns were detected by samplers positioned on different parts of the body. Chest and wrist samplers were the most similar with correlations identified for 20% of chemical exposures (Spearman's Rho > 0.8, p < 0.05). In contrast, the greatest differences were found for head and foot samplers with the weakest correlations across evaluated exposures (8% compounds, Spearman's Rho > 0.8, p < 0.05). SIGNIFICANCE: The placement of wearable passive air samplers influences the exposures captured and should be considered in future exposure and epidemiological studies. IMPACT STATEMENT: Traditional approaches for assessing personal exposure to airborne contaminants with active samplers presents challenges due to their cost, size, and weight. Wearable passive samplers have recently emerged as a non-invasive, lower cost tool for measuring environmental exposures. While these samplers can be worn on different parts of the body, their position can influence the type of exposure that is captured. This study comprehensively evaluates the exposure to airborne chemical contaminants measured at different passive sampler positions worn on the head, chest, wrist, and foot. Findings provide guidance on sampler placement based on chemicals and emission sources of interest.