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Polycyclic aromatic compounds (PACs) in Canadian air and deposition were examined at the national scale for the first time in over twenty-five years. Air concentrations spanned four orders of magnitude, and were highest near industrial emitters and lowest in the Arctic. Declines in unsubstituted PAHs were observed at locations close to industrial facilities that had reduced emissions, but trends elsewhere were modest or negligible. Retene concentrations are increasing at several locations. Ambient concentrations of benzo[a]pyrene exceeded Ontario's health-based guideline in many urban/industrial areas. The estimated toxicity of the ambient PAC mixture increased by up to a factor of six when including compounds beyond the US EPA PAHs. Knowledge of PAC deposition is limited to the Laurentian Great Lakes and Athabasca Oil Sands regions. The atmosphere remained a net source of PAHs to the Great Lakes, though atmospheric inputs were decreasing with halving times of 26-30 years. Chemical transport modelling substantially overestimated wet deposition, but model performance is unknown for dry deposition. Sources from Asia, Europe and North America contributed to Arctic and Sub-Arctic concentrations, whereas transboundary or long-range transport have not been assessed outside Canada's north. Climate-related impacts from re-emission and forest fires were implicated in maintaining air concentrations in the high Arctic that were not consistent with global emissions reductions. Industrial emission decreases were substantial at the national scale, but their influence on the environment was limited to areas near relevant facilities. When examined through the lens of ambient levels at the local scale, evidence suggested that contributions from residential wood combustion and motor vehicles were smaller and larger, respectively, than those reported in national inventories. Future work aimed at characterizing PACs beyond the EPA PAHs, improving measurement coverage, elucidating deposition phenomena, and refining estimates of source contributions would assist in reducing remaining knowledge gaps about PACs in Canada., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2020. Published by Elsevier Ltd. All rights reserved.)

Twenty-five years after the first look at polycyclic aromatic compounds (PACs) in Canada, this article presents current knowledge on Canadian PAC emission sources. The analysis is based on national inventories (the National Pollutant Release Inventory (NPRI) and the Air Pollutant Emissions Inventory (APEI)), an analysis of Canadian forest fires, and several air quality model-ready emissions inventories. Nationally, forest fires continue to dominate PAC emissions in Canada, however there is uncertainty in these estimates. Though forest fire data show a steady average in the total annual area burned historically, an upward trend has developed recently. Non-industrial sources (home firewood burning, mobile sources) are estimated to be the second largest contributor (∼6-8 times lower than forest fires) and show moderate decreases (25%-65%) in the last decades. Industrial point sources (aluminum production, iron/steel manufacturing) are yet a smaller contributor and have seen considerable reductions (90% +) in recent decades. Fugitive emissions from other industrial sources (e.g. disposals by the non-conventional oil extraction and wastewater sectors, respectively) remain a gap in our understanding of total PAC emissions in Canada. Emerging concerns about previously unrecognized sources such as coal tar-sealed pavement run-off, climate change are discussed elsewhere in this special issue. Results affirm that observations at the annual/national scale are not always reflective of regional/local or finer temporal scales. When determining which sources contribute most to human and ecosystem exposure in various contexts, examination at regional and local scales is needed. There is uncertainty overall in emissions data stemming in part from various accuracy issues, limitations in the scope of the various inventories, and inventory gaps, among others., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2020. Published by Elsevier Ltd. All rights reserved.)

In this review, global change processes have been linked to polycyclic aromatic compounds (PACs) in Canada and a first national budget of sources and sinks has been derived. Sources are dominated by wildfire emissions that affect western and northern regions of Canada disproportionately due to the location of Pacific and boreal forests and the direction of prevailing winds. Wildfire emissions are projected to increase under climate warming along with releases from the thawing of glaciers and permafrost. Residential wood combustion, domestic transportation and industry contribute the bulk of anthropogenic emissions, though they are substantially smaller than wildfire emissions and are not expected to change considerably in coming years. Other sources such as accidental spills, deforestation, and re-emission of previous industrial deposition are expected to contribute anthropogenic and biogenic PACs to nearby ecosystems. PAC sinks are less well-understood. Atmospheric deposition is similar in magnitude to anthropogenic sources. Considerable knowledge gaps preclude the estimation of environmental transformations and transboundary flows, and assessing the importance of climate change relative to shifts in population distribution and energy production is not yet possible. The outlook for PACs in the Arctic is uncertain due to conflicting assessments of competing factors and limited measurements, some of which provide a baseline but have not been followed up in recent years. Climate change has led to an increase in primary productivity in the Arctic Ocean, but PAC-related impacts on marine biota appear to be modest. The net effect of changes in ecological exposure from changing emissions and environmental conditions throughout Canada remains to be seen. Evidence suggests that the PAC budget at the national scale does not represent impacts at the local or regional level. The ability to assess future trends depends on improvements to Canada's environmental measurement strategy and biogeochemical modelling capability., Competing Interests: Declaration of competing interest The authors declare no conflicts of interest., (Crown Copyright © 2021. Published by Elsevier Ltd. All rights reserved.)

A wide variety of sampling techniques and strategies are needed to analyze polycyclic aromatic compounds (PACs) and interpret their distributions in various environmental media (i.e., air, water, snow, soils, sediments, peat and biological material). In this review, we provide a summary of commonly employed sampling methods and strategies, as well as a discussion of routine and innovative approaches used to quantify and characterize PACs in frequently targeted environmental samples, with specific examples and applications in Canadian investigations. The pros and cons of different analytical techniques, including gas chromatography - flame ionization detection (GC-FID), GC low-resolution mass spectrometry (GC-LRMS), high performance liquid chromatography (HPLC) with ultraviolet, fluorescence or MS detection, GC high-resolution MS (GC-HRMS) and compound-specific stable (δ 13 C, δ 2 H) and radiocarbon (Δ 14 C) isotope analysis are considered. Using as an example research carried out in Canada's Athabasca oil sands region (AOSR), where alkylated polycyclic aromatic hydrocarbons and sulfur-containing dibenzothiophenes are frequently targeted, the need to move beyond the standard list of sixteen EPA priority PAHs and for adoption of an AOSR bitumen PAC reference standard are highlighted., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2020. Published by Elsevier Ltd. All rights reserved.)