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The US. EnvironmentalProtection Agency (EPA) initiated the national PM2.5 Chemical Speciation Monitoring Network (CSN) in 2000 to support evaluation of long-term trends and to better quantify the impact of sources on particulate matter (PM) concentrations in the size range below 2.5 μm aerodynamic diameter (PM2.5; fine particles). The network peaked at more than 260 sites in 2005. In response to the 1999 Regional Haze Rule and the need to better understand the regional transport of PM, EPA also augmented the long-existing Interagency Monitoring of Protected Visual Environments (IMPROVE) visibility monitoring network in 2000, adding nearly 100 additional IMPROVE sites in rural Class 1 Areas across the country. Both networks measure the major chemical components of PM2.5 using historically accepted filter-based methods. Components measured by both networks include major anions, carbonaceous material, and a series of trace elements. CSN also measures ammonium and other cations directly, whereas IMPROVE estimates ammonium assuming complete neutralization of the measured sulfate and nitrate. IMPROVE also measures chloride and nitrite. In general, the field and laboratory approaches used in the two networks are similar; however, there are numerous, often subtle differences in sampling and chemical analysis methods, shipping, and quality control practices. These could potentially affect merging the two data sets when used to understand better the impact of sources on PM concentrations and the regional nature and long-range transport of PM2zs. This paper describes, for the first time in the peer-reviewed literature, these networks as they have existed since 2000, outlines differences infield and laboratory approaches, provides a summary of the analytical parameters that address data uncertainty, and summarizes major network changes since the inception of CSN. Implications: Two long-term chemical speciation particle monitoring networks have operated simultaneously in the United States since 2001, when the EPA began regular operations of its PM2.5 Chemical Speciation Monitoring Network (IMPROVE began in 1988). These networks use similar field sampling and analytical methods, but there are numerous, often subtle differences in equipment and methodologies that can affect the results. This paper describes these networks since 20000 (inception of CSN) and their differences, and summarizes the analytical parameters that address data uncertainty, providing researches and policymakers with background information they may need (e.g., for 2018 PM2.5 designation and State Implementation Plan process; McCarthy, 2013) to assess results from each network and decide how these data sets can be mutually employed for enhanced analyses. Changes in CSN and IMPROVE that have occurred over the years also are described.

Unlabelled: A year-long study was conducted in Pinal County, AZ, to characterize coarse (2.5 - 10 microm aerodynamic diameter, AD) and fine (< 2.5 microm AD) particulate matter (PMc and PMf, respectively) to further understand spatial and temporal variations in ambient PM concentrations and composition in rural, arid environments. Measurements of PMc and PMf mass, ions, elements, and carbon concentrations at one-in-six day resolution were obtained at three sites within the region. Results from the summer of 2009 and specifically the local monsoon period are presented. The summer monsoon season (July - September) and associated rain and/or high wind events, has historically had the largest number of PM10 NAAQS exceedances within a year. Rain events served to clean the atmosphere, decreasing PMc concentrations resulting in a more uniform spatial gradient among the sites. The monsoon period also is characterized by high wind events, increasing PMc mass concentrations, possibly due to increased local wind-driven soil erosion or transport. Two PM10 NAAQS exceedances at the urban monitoring site were explained by high wind events and can likely be excluded from PM10 compliance calculations as exceptional events. At the more rural Cowtown site, PM10 NAAQS exceedances were more frequent, likely due to the impact from local dust sources. PM mass concentrations at the Cowtown site were typically higher than at the Pinal County Housing and Casa Grande sites. Crustal material was equal to 52-63% of the PMc mass concentration on average. High concentrations of phosphate and organic carbon found at the rural Cowtown were associated with local cattle feeding operations. A relatively high correlation between PMc and PMf (R2 = 0.63) indicated that the lower tail of the coarse particle fraction often impacts the fine particle fraction, increasing the PMf concentrations. Therefore, reductions in PMc sources will likely also reduce PMf concentrations, which also are near the value of the 24-hr PM2.5 NAAQS., Implications: In the desert southwest, summer monsoons are often associated with above average PM10 (< 10 microm AD) mass concentrations. Competing influences of monsoon rain and wind events showed that rain suppresses ambient concentrations while high wind increase them. In this region, the PMc fraction dominates PM10 and crustal sources contribute 52-63% to local PMc mass concentrations on average. Cattle feedlot emissions are also an important source and a unique chemical signature was identified for this source. Observations suggest monsoon wind events alone cannot explain PM10 NAAQS exceedances, thus requiring these values to remain in compliance calculations rather than being removed as exceptional wind events.

Sampling and handling artifacts can bias filter-based measurements of particulate organic carbon (OC). Several measurement-based methods for OC artifact reduction and/or estimation are currently used in research-grade field studies. OC frequently is not artifact-corrected in large routine sampling networks (e.g., U.S. Environmental Protection Agency (EPA)'s Chemical Speciation Network). In some cases, the OC artifact has been corrected using a regression method (RM) for artifact estimation. In this method, the gamma-intercept of the regression of the OC concentration on the fine particle (PM2.5) mass concentration is taken to be an estimate of the average OC sampling artifact (net of positive and negative artifacts). This paper discusses options for artifact correction in large routine sampling networks. Specifically, the goals are to (1) articulate the assumptions and limitations inherent to the RM, (2) describe other artifact correction approaches, and (3) suggest a cost-effective method for artifact correction in large monitoring networks. The RM assumes a linear relationship between measured OC and PM mass: a constant slope (OC mass fraction) and a constant intercept (RM artifact estimate). These assumptions are not always valid. Additionally, outliers and other individual data points can have a large influence on the RM artifact estimates. The RM yields results within the range of measurement-based methods for some datasets and not for others. Given that the adsorption of organic gases increases with atmospheric concentrations of organics, subtraction of an average artifact from all samples (e.g., across multiple sites) will underestimate OC for lower-concentration samples (e.g., clean sites) and overestimate OC for higher-concentration samples (e.g., polluted sites). For relatively accurate, simple, and cost-effective artifact OC estimation in large networks, the authors suggest backup filter sampling on at least 10% of sampling days at all sites with artifact correction on a sample-by-sample basis as described herein.

Secondary aerosols comprise a major fraction of fine particulate matter (PM2.5) in all parts of the country, during all seasons, and times of day. The most abundant secondary species include sulfate, nitrate, ammonium, and secondary organic aerosols (SOAs). The relative abundance of each species varies in space and time as a function of meteorology, source emissions strength and type, thermodynamics, and atmospheric processing. Transport of secondary aerosols from upwind locations can contribute significantly at downwind receptor sites, especially regionally in the eastern United States, and across a given urbanized area, such as in Los Angeles. Processes governing the formation of the inorganic secondary species (sulfate, nitrate, and ammonium) are fairly well understood, although the occurrence of nucleation bursts initiated with the formation of ultrafine sulfuric acid particles observed regionally on clean days in the eastern United States was unexpected. Because of the complex nature of organic material in air, much is still to be learned about the sources, formation, and even spatial and temporal distributions of SOAs. For example, a considerable fraction of ambient organic PM is oxidized organic species, many of which still need to be identified, quantified, and their sources and formation mechanisms determined. Furthermore, significant uncertainty (approaching 50% or more) is associated with estimating the SOA fraction of organic material in air with current methods. This review summarizes the findings of the Supersites Program and related studies addressing secondary particulate matter (PM), including spatial and temporal variations of secondary PM and its precursor species, data and methods for determining the primary and secondary fractions of PM mass, and findings on the anthropogenic and natural fractions of secondary PM.

The U.S. Environmental Protection Agency (EPA) established the Particulate Matter (PM) Supersites Program to provide key stakeholders (government and private sector) with significantly improved information needed to develop effective and efficient strategies for reducing PM on urban and regional scales. All Supersites projects developed and evaluated methods and instruments, and significant advances have been made and applied within these programs to yield new insights to our understanding of PM accumulation in air as well as improved source-receptor relationships. The tested methods include a variety of continuous and semicontinuous instruments typically with a time resolution of an hour or less. These methods often overcome many of the limitations associated with measuring atmospheric PM mass concentrations by daily filter-based methods (e.g., potential positive or negative sampling artifacts). Semicontinuous coarse and ultrafine mass measurement methods also were developed and evaluated. Other semicontinuous monitors tested measured the major components of PM such as nitrate, sulfate, ammonium, organic and elemental carbon, trace elements, and water content of the aerosol as well as methods for other physical properties of PM, such as number concentration, size distribution, and particle density. Particle mass spectrometers, although unlikely to be used in national routine monitoring networks in the foreseeable future because of their complex technical requirements and cost, are mentioned here because of the wealth of new information they provide on the size-resolved chemical composition of atmospheric particles on a near continuous basis. Particle mass spectrometers likely represent the greatest advancement in PM measurement technology during the last decade. The improvements in time resolution achieved by the reported semicontinuous methods have proven to be especially useful in characterizing ambient PM, and are becoming essential in allowing scientists to investigate sources of particulate pollution and to probe into the dynamics and mechanisms of aerosol formation in the atmosphere.

In 1998, the U.S. Environmental Protection Agency (EPA) initiated a major air quality program known as the Particulate Matter (PM) Supersites Program. The Supersites Program was a multiyear, $27 million air quality monitoring program consisting of eight regional air quality projects located throughout the United States, each with differing atmospheric pollution conditions resulting from variations in source emissions and meteorology. The overall goal of the program was to elucidate source-receptor relationships and atmospheric processes leading to PM accumulation on urban and regional scales; thus providing the scientific underpinning for modeling and data analysis efforts to support State Implementation Plans and more effective risk management approaches for PM. The program had three main objectives: (1) conduct methods development and evaluation, (2) characterize ambient PM, and (3) support health effects and exposure research. This paper provides a synthesis of key scientific findings from the Supersites Program and related studies. EPA developed 16 science/policy-relevant questions in conjunction with state and other federal agencies, Regional Planning Organizations, and the private sector. These questions were addressed to the extent possible, even given the vast amount of new information available from the Supersites Program, in a series of papers published as a special issue of the Journal of Air & Waste Management Association (February 2008). This synthesis also includes discussions of: (1) initial Supersites Program support for air quality management efforts in specific locations throughout the United States; (2) selected policy-relevant insights, based on atmospheric sciences findings, useful to air quality managers and decision makers planning emissions management strategies to address current and future PM National Ambient Air Quality Standards (NAAQS) and network planning and implementation; (3) selected health-relevant insights interpreted from atmospheric sciences findings in light of future directions for health and exposure scientists planning studies of the effects of PM on human health; and (4) selected knowledge gaps to guide future research. Finally, given the scope and depth of research and findings from the Supersites Program, this paper provides a reference source so readers can glean a general understanding of the overall research conducted and its policy-relevant insights. Supporting details for the results presented are available through the cited references. An annotated table of contents allows readers to easily find specific subject matter within the text.

The Nigerian city of Lagos experiences severe air pollution as a result of emissions and subsequent atmospheric photochemistry and aerosol chemistry. A year-long study, between August 2020 and July 2021, included measurements of gas-phase and aerosol processes, with surface meteorology at six urban sites. The sites were selected to represent near seacoast conditions, urban sites, and inland locations near agricultural and grassland ecosystems. The observations included continuous concentrations for CO, SO2, NOx, O3, PM2.5, and PM10. Samples were collected and analyzed for speciated volatile organic compounds (VOCs) and particulate chemical composition including inorganic and organic chemical species. The average diel variations in concentrations indicated well-known local photochemistry resulting from the presence of combustion sources, including motor vehicles, petroleum production and use, and open burning. The annual diel characteristics were emission-dependent and were modulated by meteorological variability, including the sea breeze and the seasonal changes associated with monsoons and Harmattan winds. Gases and particulate matter varied daily, consistent with the onset of source activities during the day. Fine particles less than 2.5 μm in diameter (PM2.5) included both primary particles from emission sources and secondary particles produced in the atmosphere by photochemical reactions. Importantly, particle sources included a large component of dust and carbonaceous material. For the latter, there was evidence that particle concentrations were dominated by primary sources, with little secondary material formed in the atmosphere. From complementary measurements, there were occasions when regional chemical processes affected the local conditions, including transportation, industry, commercial activity, and open waste burning. [ABSTRACT FROM AUTHOR]

The U.S. Environmental Protection Agency (EPA) initiated the national PM2.5Chemical Speciation Monitoring Network (CSN) in 2000 to support evaluation of long-term trends and to better quantify the impact of sources on particulate matter (PM) concentrations in the size range below 2.5 μm aerodynamic diameter (PM2.5; fine particles). The network peaked at more than 260 sites in 2005. In response to the 1999 Regional Haze Rule and the need to better understand the regional transport of PM, EPA also augmented the long-existing Interagency Monitoring of Protected Visual Environments (IMPROVE) visibility monitoring network in 2000, adding nearly 100 additional IMPROVE sites in rural Class 1 Areas across the country. Both networks measure the major chemical components of PM2.5using historically accepted filter-based methods. Components measured by both networks include major anions, carbonaceous material, and a series of trace elements. CSN also measures ammonium and other cations directly, whereas IMPROVE estimates ammonium assuming complete neutralization of the measured sulfate and nitrate. IMPROVE also measures chloride and nitrite. In general, the field and laboratory approaches used in the two networks are similar; however, there are numerous, often subtle differences in sampling and chemical analysis methods, shipping, and quality control practices. These could potentially affect merging the two data sets when used to understand better the impact of sources on PM concentrations and the regional nature and long-range transport of PM2.5. This paper describes, for the first time in the peer-reviewed literature, these networks as they have existed since 2000, outlines differences in field and laboratory approaches, provides a summary of the analytical parameters that address data uncertainty, and summarizes major network changes since the inception of CSN.ImplicationsTwo long-term chemical speciation particle monitoring networks have operated simultaneously in the United States since 2001, when the EPA began regular operations of its PM2.5 Chemical Speciation Monitoring Network (IMPROVE began in 1988). These networks use similar field sampling and analytical methods, but there are numerous, often subtle differences in equipment and methodologies that can affect the results. This paper describes these networks since 2000 (inception of CSN) and their differences, and summarizes the analytical parameters that address data uncertainty, providing researchers and policymakers with background information they may need (e.g., for 2018 PM2.5 designation and State Implementation Plan process; McCarthy, 2013) to assess results from each network and decide how these data sets can be mutually employed for enhanced analyses. Changes in CSN and IMPROVE that have occurred over the years also are described. [ABSTRACT FROM AUTHOR]

A current re-engineering of the United States routine ambient monitoring networks intended to improve the balance in addressing both regulatory and scientific objectives is addressed in this paper. Key attributes of these network modifications include the addition of collocated instruments to produce multiple pollutant characterizations across a range of representative urban and rural locations in a new network referred to as the National Core Monitoring Network (NCore). The NCore parameters include carbon monoxide (CO), sulfur dioxide (SO2), reactive nitrogen (NOy), ozone (O3), and ammonia (NH3) gases and the major fine particulate matter (PM2.5) aerosol components (ions, elemental and organic carbon fractions, and trace metals). The addition of trace gas instruments, deployed at existing chemical speciation sites and designed to capture concentrations well below levels of national air quality standards, is intended to support both long-term epidemiological studies and regional-scale air quality model evaluation. In addition to designing the multiple pollutant NCore network, steps were taken to assess the current networks on the basis of spatial coverage and redundancy criteria, and mechanisms were developed to facilitate incorporation of continuously operating particulate matter instruments. [ABSTRACT FROM AUTHOR]

Abstract: We present the design and fabrication of a micro electro mechanical systems (MEMS) air-microfluidic particulate matter (PM) sensor, and show experimental results obtained from exposing the sensor to concentrations of tobacco smoke and diesel exhaust, two commonly occurring PM sources. Our sensor measures only 25mm×21mm×2mm in size and is two orders of magnitude smaller than commercially available direct mass PM sensors. The small shape allows our sensor to be used for continuous recording of personal PM exposure levels. The sensor contains an air-microfluidic circuit that separates the particles by size (virtual impactor) and then transports and deposits the selected particles using thermophoretic precipitation onto the surface of a microfabricated mass-sensitive film bulk acoustic resonator (FBAR). The mass-loading of the FBAR causes a change in its resonant frequency, and the rate of the frequency change corresponds to the particle concentration in the sampled air volume. We present experimental results that demonstrate the performance of our sensor for measuring PM mass emitted from diesel exhaust and tobacco smoke, and show that it exhibits sensitivity approaching 2μg/m3 with up to 10min integration time. [Copyright &y& Elsevier]

Dust storms are significant contributors to ambient levels of particulate matter (PM) in many areas of the world. Central Asia, an area that is relatively understudied in this regard, is anticipated to be affected by dust storms due to its proximity to several major deserts that are in and generally surround Central Asia (e.g., the Aral Sea region, the Taklimakan desert in Western China). To investigate the relative importance of mineral dust (dust specifically composed of soil related minerals and oxides) in Central Asia, PM 10 and PM 2.5 , and by difference, coarse particles (particles with diameters between 2.5 and 10 μm) were measured at two sites, Bishkek and Lidar Station Teplokluchenka (Lidar), in the Kyrgyz Republic. Samples were collected every other day from July 2008 to July 2009. Daily samples were analyzed for mass and organic and elemental carbon. Samples were also composited on a bi-weekly basis and analyzed for elemental constituents and ionic components. In addition, samples collected on days with relatively high and low PM concentrations were analyzed before, and separately, from the biweekly composites to investigate the chemical differences between the episodic events. Data from the episodic samples were averaged into the composited averages. Using the elemental component data, several observational models were examined to estimate the contribution of mineral dust to ambient PM levels. A mass balance was also conducted. Results indicate that at both sites, mineral dust (as approximated by the “dust oxide” model) and organic matter (OM) were the dominant contributors to PM 10 and PM 2.5 . Mineral dust was a more significant contributor to the coarse PM (PM 10-2.5 ) during high event samples at both sites, although the relative contribution is greater at the Lidar site (average ± standard deviation = 42 ± 29%) as compared with the Bishkek site (26 ± 16%). Principal Components Analysis (PCA) was performed using data from both sites, and PCA indicated that mineral dust explained the majority of the variance in PM concentrations, and that the major apportioned factors of PM 10 and PM 2.5 were chemically similar between sites. [ABSTRACT FROM AUTHOR]

Abstract: Central Asia is a relatively understudied region of the world in terms of characterizing ambient particulate matter (PM) and quantifying source impacts of PM at receptor locations, although it is speculated to have an important role as a source region for long-range transport of PM to Eastern Asia, the Pacific Ocean, and the Western United States. PM is of significant interest not only because of its adverse effect on public health but also due to its more recently realized role in climate change. To investigate the sources and characteristics of PM in the region, a series of PM2.5 and PM10 samples were collected on an every-other-day basis at two sites (termed “Bishkek” and “Teploklyuchenka”) in the Central Asian nation of the Kyrgyz Republic (also known as Kyrgyzstan) for a full year from July 2008 to July 2009. These samples were analyzed using standard methods for mass, organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), water-insoluble organic carbon by difference (OC minus WSOC) and a variety of molecular marker chemical species to be used in a chemical mass balance (CMB) model to apportion the sources of OC. These analyses indicate that approximately 19 ± 6.4% of the PM2.5 mass at both sites throughout the year consists of OC. The carbonaceous component of PM2.5 is dominated by OC, with OC/Total Carbon (TC) ratios being around 0.8 in the winter to almost 0.95 in the summer months. The CMB analysis indicated that mobile sources, i.e., gasoline and diesel engine exhaust, biomass combustion, and biogenic secondary organic aerosol (SOA) formation from isoprene and α-pinene precursors in the summer months were the dominant sources of OC. A strong positive correlation was observed between non-biomass burning WSOC and the un-apportioned OC from the CMB analysis, indicating that some of this un-apportioned OC is WSOC and likely the result of SOA-forming atmospheric processes that were not estimated by the CMB analysis performed. In addition, a comparison of the predominant contributors to OC between the two sites indicates that biomass combustion is a stronger relative source of OC at the Teploklyuchenka site, particularly in the winter, while contributions of isoprene- and α-pinene-derived SOA to the measured OC was relatively similar between the sites. [Copyright &y& Elsevier]

Abstract: This study presents the development and field evaluation of a compact high-volume dichotomous sampler (HVDS) that collects coarse and fine particulate matter. The key features of this device is the utilization of a round nozzle virtual impactor with a 50% cutpoint at aerodynamic diameter, operating at a high inlet flow rate with a calculated Reynolds number of approximately . In its primary configuration as tested, the sampler size-fractionates into coarse and fine fractions with a minor flow ratio of 10% (minor/total flow rate), with major and minor flow rates of 900 and , respectively. Performance evaluation for concentration enrichment was conducted with a 4% minor flow ratio ( minor flow) as well. Tests demonstrated near ideal results at both 10% and 4% minor flow ratios, indicating enrichment to be independent of minor flow rates within the range evaluated. Reasonable agreement was found between the new sampler and collocated Partisol and MOUDI for ambient measurements. A tandem virtual impactor super-concentration system was also tested with the virtual impactor followed by a round nozzle virtual impactor and proved to be an efficient system to achieve higher concentration enrichment of ambient particles up to 180 times ambient levels. Investigation of the effect of different ambient parameters like RH and wind speed on coarse PM concentration corroborates results from earlier studies. The HVDS is an effective system to collect coarse and fine PM simultaneously, allowing for comprehensive standard chemical analyses over short sampling intervals. [Copyright &y& Elsevier]