Search

Abstract: Multiyear (2000–2006) seasonal measurements of carbon monoxide, hydrocarbons, halogenated species, dimethyl sulfide, carbonyl sulfide and C1–C4 alkyl nitrates at the South Pole are presented for the first time. At the South Pole, short-lived species (such as the alkenes) typically were not observed above their limits of detection because of long transit times from source regions. Peak mixing ratios of the longer lived species with anthropogenic sources were measured in late winter (August and September) with decreasing mixing ratios throughout the spring. In comparison, compounds with a strong oceanic source, such as bromoform and methyl iodide, had peak mixing ratios earlier in the winter (June and July) because of decreased oceanic production during the winter months. Dimethyl sulfide (DMS), which is also oceanically emitted but has a short lifetime, was rarely measured above 5 pptv. This is in contrast to high DMS mixing ratios at coastal locations and shows the importance of photochemical removal during transport to the pole. Alkyl nitrate mixing ratios peaked during April and then decreased throughout the winter. The dominant source of the alkyl nitrates in the region is believed to be oceanic emissions rather than photochemical production due to low alkane levels. Sampling of other tropospheric environments via a Twin Otter aircraft included the west coast of the Ross Sea and large stretches of the Antarctic Plateau. In the coastal atmosphere, a vertical gradient was found with the highest mixing ratios of marine emitted compounds at low altitudes. Conversely, for anthropogenically produced species the highest mixing ratios were measured at the highest altitudes, suggesting long-range transport to the continent. Flights flown through the plume of Mount Erebus, an active volcano, revealed that both carbon monoxide and carbonyl sulfide are emitted with an OCS/CO molar ratio of 3.3 × 10−3 consistent with direct observations by other investigators within the crater rim. [Copyright &y& Elsevier]

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Emissions and atmospheric concentrations of CH4 continue to increase, maintaining CH4 as the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the factors explaining the well-observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in-situ and greenhouse gas observing satellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land-surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full datasets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this edition benefits from important progress in estimating inland freshwater emissions, with better accounting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double accounting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double accounting that still exists (average of 23 Tg CH4 yr-1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr-1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr-1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr-1 or ~65 % are attributed to direct anthropogenic sources in the fossil, agriculture and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr-1or 63–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr-1 (range 9–40). Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr-1) larger global emissions (669 Tg CH4 yr-1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr-1 in Saunois et al. (2016, 2020), respectively), and for the first time uncertainty in bottom-up and top-down budgets overlap. The latitudinal distribution from atmospheric inversion-based emissions indicates a predominance of tropical and southern hemisphere emissions (~65 % of the global budget, <30° N) compared to mid (30° N–60° N, ~30 % of emissions) and high-northern latitudes (60° N–90° N, ~4 % of global emissions). This latitudinal distribution is similar in the bottom-up budget though the bottom-up budget estimates slightly larger contributions for the mid and high-northern latitudes, and slightly smaller contributions from the tropics and southern hemisphere than the inversions. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. We identify five major priorities for improving the CH4 budget: i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; ii) further development of process-based models for inland-water emissions; iii) intensification of CH4 observations at local (e.g., FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; iv) improvements of transport models and the representation of photochemical sinks in top-down inversions, and v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024). [ABSTRACT FROM AUTHOR]

Reports on the effect of liquefied petroleum gas (LPG) leakage to the atmosphere of Mexico City, Mexico. Dominant nonmethane hydrocarbons (NMHC) in the city's atmosphere; High concentration of NMHCs; Collection of samples; Composition of LPG used in the city.

Presents research which estimated the atmospheric residence time for methyl bromide (CH3Br). Use of Junge's 1963 general proposal; Methyl bromide in the atmosphere; Its sources; Consistency of findings with previous research.

NASA's Student Airborne Research Program (SARP) has completed 13 years of airborne student research since its inception in 2009. The 8-week summer internship program provides students, typically rising undergraduate seniors, with an opportunity to get hands-on experience in making Earth system measurements using NASA's airborne science platforms. Students also make complementary surface-based measurements, analyze airborne and surface data in the context of related data (e.g. coincident satellite measurements or prior-year SARP data), and present results to peers, program leadership, agency management, and the community. The program splits its time between the NASA Armstrong flight facility in Palmdale, California, and the University of California, Irvine. It is implemented with participation of faculty advisors (who provide many of the instruments used) and graduate student mentors, under the overall leadership of the NASA Earth Science Division. Disciplinary foci include atmospheric gases and aerosols, ocean biology, and terrestrial ecology using both in situ and remote sensing instruments. Students are also taken on site visits to nearby laboratories and facilities and attend lectures from visiting faculty and NASA agency personnel. The program engages approximately 30 students per year, with overall approximate gender balance. The program has a high rate of STEM retention, and its alumni are actively engaged in graduate and postgraduate programs in Earth system science and other disciplines. A summary of scientific and programmatic outcomes and a description of how the program has evolved will be presented. [ABSTRACT FROM AUTHOR]

In this study, the WRF-Chem v4.4 model was utilized to evaluate the sensitivity of O 3 simulations with three bottom-up emission inventories (EDGAR-HTAP v2 and v3 and KORUS v5) using surface and aircraft data in East Asia during the Korea-United States Air Quality (KORUS-AQ) campaign period in 2016. All emission inventories were found to reproduce the diurnal variations of O 3 and its main precursor NO 2 as compared to the surface monitor data. However, the spatial distributions of the daily maximum 8 h average (MDA8) O 3 in the model do not completely align with the observations. The model MDA8 O 3 had a negative (positive) bias north (south) of 30° N over China. All simulations underestimated the observed CO by 50 %–60 % over China and South Korea. In the Seoul Metropolitan Area (SMA), EDGAR-HTAP v2 and v3 and KORUS v5 simulated the vertical shapes and diurnal patterns of O 3 and other precursors effectively, but the model underestimated the observed O 3 , CO, and HCHO concentrations. Notably, the model aromatic volatile organic compounds (VOCs) were significantly underestimated with the three bottom-up emission inventories, although the KORUS v5 shows improvements. The model isoprene estimations had a positive bias relative to the observations, suggesting that the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.04 overestimated isoprene emissions. Additional model simulations were conducted by doubling CO and VOC emissions over China and South Korea to investigate the causes of the model O 3 biases and the effects of the long-range transport on the O 3 over South Korea. The doubled CO and VOC emission simulations improved the model O 3 simulations for the local-emission-dominant case but led to the model O 3 overestimations for the transport-dominant case, which emphasizes the need for accurate representations of the local VOC emissions over South Korea. [ABSTRACT FROM AUTHOR]

Ports are major air pollution sources impacting downwind communities with emissions from port activities, nearby energy and other heavy industries, truck, train, and vessel traffic, and commuting traffic. The Ports of Los Angeles/Long Beach, denoted Ports, are the western hemisphere's largest, with plans for port electrification to reduce air pollution. The covid19 shutdown impacted the Ports, providing a real-world experiment on the effects of electrification on exposure to neighboring communities. Eight in situ surveys with a mobile air quality laboratory (14 trace gases, aerosols, and meteorology) were conducted spanning the covid19 shutdown to characterize the resultant air quality changes. These data were combed with time series (2015-) from six Port area air quality stations and TROPOMI satellite nitrogen dioxide NO 2 column XNO 2. In situ surveys showed dramatic NO 2 decreases from Jul. 2019 to May 2020 (during the shutdown), with NO 2 only returning towards pre-covid levels by Jul. 2022. Lesser covid19 NO 2 decreases were observed by the air quality station data and satellite XNO 2 for the Los Angeles Basin; both showed NO 2 decrease during the shutdown and an extended time for recovery to more normal concentration (and underlying economic activity) - until 2022 - far longer than the shutdown. Overall, ozone, O 3 increased, signifying that O 3 , formation is volatile organic hydrocarbons, VOH, limited, with the strongest O 3 source(s) arriving from offshore. This finding suggests efforts to purely address air quality by electrification without addressing area VOH emissions could potentially lessen, perhaps significantly, the expected air quality and health improvements in downwind communities. The Ports' area industrial sites were identified as driving these VOHs, as the inverse relationship between NO 2 and O 3 persisted during the shutdown when non-industrial VOH sources would have decreased. [Display omitted] • Mobile air quality surveyed the Los Angeles & Long Beach Ports during covid19. • Surveys, air quality station and satellite data found dramatic covid19 NO 2 decreases. • Recovery to normal pollution levels was slow - multiyear. • Ozone increased during covid19, indicating VOH-limited ozone formation. [ABSTRACT FROM AUTHOR]

Proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF-MS) is a technique commonly used to measure ambient volatile organic compounds (VOCs) in urban, rural, and remote environments. PTR-ToF-MS is known to produce artifacts from ion fragmentation, which complicates the interpretation and quantification of key atmospheric VOCs. This study evaluates the extent to which fragmentation and other ionization processes impact urban measurements of the PTR-ToF-MS ions typically assigned to isoprene (m/z 69, C 5 H 8 H +), acetaldehyde (m/z 45, CH 3 CHO +), and benzene (m/z 79, C 6 H 6 H +). Interferences from fragmentation are identified using gas chromatography (GC) pre-separation, and the impact of these interferences is quantified using ground-based and airborne measurements in a number of US cities, including Las Vegas, Los Angeles, New York City, and Detroit. In urban regions with low biogenic isoprene emissions (e.g., Las Vegas), fragmentation from higher-carbon aldehydes and cycloalkanes emitted from anthropogenic sources may contribute to m/z 69 by as much as 50 % during the day, while the majority of the signal at m/z 69 is attributed to fragmentation during the night. Interferences are a higher fraction of m/z 69 during airborne studies, which likely results from differences in the reactivity between isoprene and the interfering species along with the subsequent changes to the VOC mixture at higher altitudes. For other PTR masses, including m/z 45 and m/z 79, interferences are observed due to fragmentation and O 2+ ionization of VOCs typically used in solvents, which are becoming a more important source of anthropogenic VOCs in urban areas. We present methods to correct these interferences, which provide better agreement with GC measurements of isomer-specific molecules. These observations show the utility of deploying GC pre-separation for the interpretation PTR-ToF-MS spectra. [ABSTRACT FROM AUTHOR]

In this study, the WRF-Chem v4.4 model was utilized to evaluate three bottom-up emission inventories (EDGAR-HTAP v2, v3, and KORUS v5) using surface and aircraft data in East Asia during the Korea-United States Air Quality (KORUS-AQ) campaign period in 2016. All emission inventories were found to reproduce the diurnal variations of O3 and NO2 as compared to the surface monitor data. However, the spatial distributions of the daily maximum 8-hour average (MDA8) O3 in the model do not completely align with the observations. The model MDA8 O3 had a negative (positive) bias north (south) of 30°N over China. All simulations underestimated the observed CO by 50-60% over China and South Korea. In the Seoul Metropolitan Area (SMA), EDGAR-HTAP v2, v3, and KORUS v5 simulated the vertical shapes and diurnal patterns of O3 and other precursors effectively, but the model underestimated the observed O3, CO and HCHO concentrations. Notably, the model aromatic VOCs were significantly underestimated with the three bottom-up emission inventories, although the KORUS v5 shows improvements. The model isoprene estimations had a positive bias relative to the observations, suggesting that the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.04 overestimated isoprene emissions. Additional model simulations were conducted by doubling CO and VOC emissions over China and South Korea to investigate the causes of the model O3 biases and the effects of the long-range transport on the O3 over South Korea. The doubled CO and VOC emission simulations improved the model O3 simulations for the local emission dominant case, but led to the model O3 overestimations for the transport dominant case, which emphasizes the need for accurate representations of the local VOC emissions over South Korea. [ABSTRACT FROM AUTHOR]

Proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF-MS) is a technique commonly used to measure ambient volatile organic compounds (VOCs) in urban, rural, and remote environments. PTR-ToF-MS is known to produce artifacts from ion fragmentation, which complicates the interpretation and quantification of key atmospheric VOCs. This study evaluates the extent to which fragmentation and other ionization processes impacts urban measurements of the PTR-ToF-MS ions typically assigned to isoprene (m/z 69, C5H8H+), acetaldehyde (m/z 45, CH3CHO+), and benzene (m/z 79, C6H6H+). Interferences from fragmentation are identified using gas-chromatography (GC) pre-separation and the impact of these interferences are quantified using ground-based and airborne measurements in a number of US cities, including Las Vegas, Los Angeles, New York City, and Detroit. In urban regions with low biogenic isoprene emissions (e.g., Las Vegas), fragmentation from higher carbon aldehydes and cycloalkanes emitted from anthropogenic sources may contribute to m/z 69 by as much as 50% during the day, while the majority of the signal at m/z 69 is attributed to fragmentation during the night. Interferences are a higher fraction of m/z 69 during airborne studies, which likely results from differences in the reactivity between isoprene and the interfering species along with the subsequent changes to the VOC mixture at higher altitudes. For other PTR masses, including m/z 45 and m/z 79, interferences are observed due to the fragmentation and secondary ionization of VOCs typically used in solvents, which are becoming a more important source of anthropogenic VOCs in urban areas. We present methods to correct these interferences, which provide better agreement with GC measurements of isomer specific molecules. These observations show the utility of deploying GC pre-separation for the interpretation PTR-ToF-MS spectra. [ABSTRACT FROM AUTHOR]

Model intercomparison studies often report a large spread in simulation results, but quantifying the causes of these differences is hindered by the fact that several processes contribute to the model spread simultaneously. Here we use the Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICA) version 0 to investigate the model resolution dependencies of simulated chemical species, with a focus on the differences between global uniform grid and regional refinement grid simulations with the same modeling framework. We construct two global (ne30 [∼112 km] and ne60 [∼56 km]) and two regional refinement grids over Korea (ne30x8 [∼14 km] and ne30x16 [∼7 km]). The grid resolution can change chemical concentrations by an order of magnitude in the boundary layer, and the importance increases as the species' reactivity increases (e.g., up to 50% and 1,000% changes for ethane and xylenes, respectively). The diurnal cycle of oxidants (OH, O3, and NO3) also varies with the grid resolution, which leads to different oxidation pathways of volatile organic compounds (e.g., the fraction of monoterpenes reacting with NO3 in Seoul around midnight is 90% for ne30, but 65% for ne30x16). The models with high‐resolution grids usually do a better job at reproducing aircraft observations during the KORUS‐AQ campaign, but not always, implying compensating errors in the coarse grid simulations. For example, ozone is better reproduced by the coarse grid due to the artificial mixing of NOx. When developing new chemical mechanisms and evaluating models over urban areas, the uncertainties associated with model resolution should be considered. Plain Language Summary: A new model framework, the Multi‐Scale Infrastructure for Chemistry and Aerosols version 0 (MUSICAv0), has been developed at NCAR to enable a computationally feasible global modeling framework while still resolving chemistry at urban scales. Using the MUSICAv0 framework with different horizontal grid resolutions (∼112, ∼56, ∼14, and ∼7 km), this work examines how much horizontal grid resolution can affect simulated chemical concentrations in 3D chemistry models. Model concentrations can vary up to 10 times between ∼112 and ∼7 km grids over urban areas at the surface. On the other hand, a region‐specific emission inventory with detailed local information is essential for some chemical species, although it is generally less important than the grid resolution for many chemical species. The model with a high‐resolution grid better reproduces observations in general, but in some cases compensating errors result in better comparisons for the coarse grid. This work suggests that the effects of grid resolution should not be ignored when evaluating new chemical mechanisms and chemistry models in future studies, and high grid resolution in 3D models is needed to simulate air pollutants over urban and downwind regions. Key Points: The dependence of simulated chemical species on model resolution is quantified in a single modeling frameworkModel evaluations can be substantially affected by grid resolution, especially for urban surface and aircraft measurements at low altitudesGrid resolution strongly impacts the oxidation of volatile organic compounds through differences in diurnal variation of oxidants [ABSTRACT FROM AUTHOR]

The Satellite Coastal and Oceanic Atmospheric Pollution Experiment (SCOAPE) cruise in the Gulf of Mexico was conducted in May 2019 by NASA and the Bureau of Ocean Energy Management to determine the feasibility of using satellite data to measure air quality in a region of concentrated oil and natural gas (ONG) operations. SCOAPE addressed both technological and scientific issues related to measuring NO2 columns over the outer continental shelf. Featured were nitrogen dioxide (NO2) instruments (Pandora, Teledyne API analyzer) at Cocodrie, LA (29.26°, −90.66°), and on the Research Vessel Point Sur operating off the Louisiana coast with measurements of ozone, carbon monoxide, and volatile organic compounds (VOCs). The findings: (a) all NO2 observations revealed two atmospheric regimes over the Gulf, the first influenced by tropical air in 10–14 May, the second influenced by flow from urban areas on 15–17 May; (b) comparisons of OMI v4 and TROPOMI v1.3 TC (total column) NO2 data with shipboard Pandora NO2 column observations averaged 13% agreement with the largest difference during 15–17 May (∼20%). At Cocodrie, the satellite–Pandora agreement was ∼5%. (c) Three new‐model Pandora instruments displayed a TC NO2 precision of 0.01 Dobson Units (∼5%); (d) regions of smaller, older natural gas operations showed high methane readings from leakage; elevated VOCs were also detected. Neither satellite nor spectrometer captured the magnitude of ambient NO2 variability near ONG platforms. Given an absence of regular air quality monitoring over the Gulf of Mexico, SCOAPE data constitute a baseline against which future observations can be compared. Plain Language Summary: The Satellite Coastal and Oceanic Atmospheric Pollution Experiment (SCOAPE) cruise in the Gulf of Mexico (GOM) conducted on the Research Vessel Point Sur in May 2019 investigated the feasibility of using satellite data to measure air quality in a region of concentrated oil and natural gas (ONG) operations. SCOAPE addressed both technological and scientific issues related to measuring NO2 columns in a prototypical coastal environment. The results are as follows. First, measurements from SCOAPE demonstrated that satellite NO2 data can be used to monitor ONG activity over the GOM. Second, during SCOAPE both OMI and TROPOMI TC (total column) NO2 amounts were higher over land and sometimes the near‐shore ONG‐rich Gulf, than over deepwater regions farther offshore. This was confirmed by Pandora spectrometer "ground truth" TC NO2 data measured throughout SCOAPE on shore and on ship. Third, SCOAPE established the reliability and precision of a new generation of Pandora spectrometers. Fourth, comparisons of satellite and Pandora TC NO2 data in SCOAPE confirm previous land–water interface studies that point to limitations in satellite NO2 in coastal regions. Finally, neither satellite nor spectrometer captures the magnitude of ambient ("nose‐level") NO2 variability in a region dotted with hundreds of ONG platforms. Key Points: Shipboard Pandora NO2 columns and surface O3, NO2, CO, and volatile organic compounds (VOCs) over the Gulf of Mexico (GOM), May 2019, displayed two air quality (AQ) regimesGOM AQ was dominated by continental NO2 sources and near‐shore VOC; deepwater oil platforms were in a clean marine regimePandora and satellite total column NO2 over GOM agreed overall within 5% in clean, clear‐sky conditions along the coast and 13% over water [ABSTRACT FROM AUTHOR]

An obituary for atmospheric chemist F. Sherwood Rowland is presented.

Organosulfur compounds (OSCs) are naturally emitted via various processes involving phytoplankton and algae in marine regions, from animal metabolism, and from biomass decomposition inland. These compounds are malodorant and reactive. Their oxidation to methanesulfonic and sulfuric acids leads to the formation and growth of atmospheric particles, which are known to influence clouds and climate, atmospheric chemical processes. In addition, particles in air have been linked to negative impacts on visibility and human health. Accurate measurements of the OSC precursors are thus essential to reduce uncertainties in their sources and contributions to particle formation in air. Two different approaches, proton-transfer reaction time-offlight mass spectrometry (PTR-ToF-MS) and canister sampling coupled to gas chromatography with flame ionization detector (GC-FID), are compared for both laboratory standards (dimethyl sulfide, DMS; dimethyl disulfide, DMDS; dimethyl trisulfide, DMTS; and methanethiol, MTO) and for a complex sample. Results show that both techniques produce accurate quantification of DMS. While PTR-ToF-MS provides real-time measurements of all four OSCs individually, significant fragmentation of DMDS and DMTS occurs, which can complicate their identification in complex mixtures. Canister sampling coupled with GC-FID provides excellent sensitivity for DMS, DMDS, and DMTS. However, MTO was observed to react on metal surfaces to produce DMDS and, in the presence of hydrogen sulfide, even DMTS. Avoiding metal in sampling systems seems to be necessary for measuring all but dimethyl sulfide in air. [ABSTRACT FROM AUTHOR]

Organosulfur compounds (OSCs) are naturally emitted via various processes involving phytoplankton and algae in marine regions, from animal metabolism, and from biomass decomposition inland. These compounds are malodorant and reactive. Their oxidation to methanesulfonic and sulfuric acids leads to the formation and growth of atmospheric particles, which are known to influence clouds and climate, atmospheric chemical processes. In addition, particles in air have been linked to negative impacts on visibility and human health. Accurate measurements of the OSC precursors are thus essential to reduce uncertainties in their sources and contributions to particle formation in air. Two different approaches, proton-transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS) and canister sampling coupled to gas chromatography with flame ionization detector (GC-FID), are compared for both laboratory standards (dimethyl sulfide, DMS; dimethyl disulfide, DMDS; dimethyl trisulfide, DMTS; and methanethiol, MTO) and for a complex sample. Results show that both techniques produce accurate quantification of DMS. While PTR-ToF-MS provides real-time measurements of all four OSCs individually, significant fragmentation of DMDS and DMTS occurs, which can complicate their identification in complex mixtures. Canister sampling coupled with GC-FID provides excellent sensitivity for DMS, DMDS, and DMTS. However, MTO was observed to react on metal surfaces to produce DMDS and, in the presence of hydrogen sulfide, even DMTS. Avoiding metal in sampling systems seems to be necessary for measuring all but dimethyl sulfide in air. [ABSTRACT FROM AUTHOR]

Nighttime concentrations of the gas phase nitrate radical (NO 3 ) were successfully measured during a four week field campaign in an arid urban location, Reno Nevada, using long-path Differential Optical Absorbance Spectrometry (DOAS). While typical concentrations of NO 3 ranged from 5 to 20 ppt, elevated concentrations were observed during a wildfire event. Horizontal mixing in the free troposphere was considerable because the sampling site was above the stable nocturnal boundary layer every night and this justified a box modeling approach. Process analysis of box model simulations showed NO 3 accounted for approximately half of the loss of internal olefins, 60% of the isoprene loss, and 85% of the α-pinene loss during the nighttime hours during a typical night of the field study. The NO 3 + aldehyde reactions were not as important as anticipated. On a polluted night impacted by wildfires upwind of the sampling location, NO 3 reactions were more important. Model simulations overpredicted NO 2 concentrations for both case studies and inorganic chemistry was the biggest influence on NO 3 concentrations and on nitric acid formation. The overprediction may be due to additional NO 2 loss processes that were not included in the box model, as deposition and N 2 O 5 uptake had no significant effect on NO 2 levels. [ABSTRACT FROM AUTHOR]

A seven-year record of surface ozone measurements from Denali National Park, Alaska shows a persistent spring maximum. These data, combined with measurements of NOx, hydrocarbons, O3, and PAN from a continental site in Alaska during the spring of 1995 are used as the basis for a sensitivity study to explore tropospheric photochemistry in this region. Because of the relatively high concentrations of NOx (mean of 116, median of 91 pptv), the net tendency was for photochemical ozone production. The range of net O3 production for average conditions measured at this site during spring is between 0.96-3.9 ppbv/day depending on the assumptions used; in any case, this production must contribute to the observed springtime maximum in O3. Model calculations showed that of the anthropogenic ozone precursors, only NOx had a strong effect on the rate of ozone production; the measured concentrations of anthropogenic hydrocarbons did not significantly affect the ozone budget. Naturally produced biogenic hydrocarbons, such as isoprene, may also have a significant effect on ozone production, even at concentrations of a few 10's of pptv. An observed temperature-isoprene relationship from a boreal site in Canada indicates that isoprene may be present during the Alaskan spring. Measurements of isoprene taken during the spring of 1996 suggest that reactive biogenic hydrocarbon emissions begin before the emergence of leaves on deciduous trees and that the concentrations were sufficient to accelerate ozone production. [ABSTRACT FROM AUTHOR]

Local surface travel needs in the People's Republic of China (mainland China) have traditionally been met largely by nonpolluting bicycles. A major automobile manufacturing/importing effort has begun in thecountry over the last decade, and planning documents indicate that the Chinese may strive to acquire more than 100 million vehicles earlyin the next century. By analogy with large automotive fleets alreadyexisting in the western world, both regional and global scale pollution effects are to be expected from the increase. The present work adopts the latest projections of Chinese automobile manufacture and performs some quantitative assessments of the extent of pollution generation. Focus for the investigation is placed upon the oxidant ozone. Emissions of the precursor species nitrogen oxides and volatile organics are constructed based on data for the current automotive sector inthe eastern portion of the United States. Ozone production is first estimated from measured values for continental/oceanic scale yields relative to precursor oxidation. The estimates are then corroborated through idealized two dimensional modeling of the photochemistry taking place in springtime air flow off the Asian land mass and toward thePacific Ocean. The projected fleet sizes could increase coastal and remote oceanic ozone concentrations by tens of parts per billion (ppb) in the lower troposphere. Influences on the tropospheric aerosol system and on the major greenhouse gas carbon dioxide are treated peripherally. Nitrogen oxides created during the vehicular internal combustion process will contribute to nitrate pollution levels measured in the open Pacific. The potential for soot and fugitive dust increases should be considered as the automotive infrastructure develops. Sincethe emerging Chinese automotive transportation system will representa substantial addition to the global fleet and all the carbon in gasoline is eventually oxidized completely, a significant rise in globalcarbon [ABSTRACT FROM AUTHOR]

Urban air pollution is rapidly becoming a major environmental problem of public concern in several developing countries of the world. Jeddah, the second-largest city in Saudi Arabia, is subject to high air pollution that has severe implications for the health of the exposed population. Fine particulate matter (PM2.5) samples were collected for 24 h daily, during a 1-year campaign from 2013 to 2014. This study presents a detailed investigation of PM2.5 mass, chemical composition, and sources covering all four seasons of the year. Samples were analyzed for black carbon (BC), trace elements (TEs), and water-soluble ionic species (IS). The chemical compositions were statistically examined, and the temporal and seasonal patterns were characterized using descriptive analysis, correlation matrices, and elemental enrichment factor (EF). Source apportionment and source locations were performed on PM2.5 samples using the positive matrix factorization (PMF) model, elemental enrichment factor, and air-mass back trajectory analysis. The 24-h mean PM2.5 and BC concentrations ranged from 33.9 ± 9.1–58.8 ± 25 µg/m3 and 1.8 ± 0.4–2.4 ± 0.6 µg/m3, respectively. Atmospheric PM2.5 concentrations were well above the 24-h WHO guideline of 15 µg/m3, with overall results showing significant temporal and seasonal variability. EF defined two broad categories of TEs: anthropogenic (Ni, V, Cu, Zn, Cl, Pb, S, Lu, and Br), and earth-crust derived (Al, Si, Mg, K, Ca, Ti, Cr, Mn, Fe, and Sr). The five identified factors resulting from PMF were (1) fossil-fuels/oil combustion (45.3%), (2) vehicular emissions (19.1%), (3) soil/dust resuspension (15.6%), (4) industrial mixed dust (13.5%), and (5) sea-spray (6.5%). This study highlights the importance of focusing control strategies, not only on reducing PM concentration but also on the reduction of components of the PM as well, to effectively protect human health and the environment. [ABSTRACT FROM AUTHOR]

Organic aerosols (OA) represent a significant fraction of total submicron particulate matter (PM1) concentrations globally, including densely populated megacities such as Seoul. However, scientific understanding of the atmospheric formation and removal processes of OA, especially for secondary organic aerosols (SOA), is still highly uncertain. In this study, we examine the characteristics of SOA formation in Seoul during spring‐summer 2016 and fall‐winter 2017/2018, using airborne and ground observations along with a 3‐D global chemical transport model, GEOS‐Chem. We use four different SOA schemes in the model, including simplified and complex volatility‐based frameworks, and evaluate them by comparing the simulations with the observations to examine how our scientific understanding embedded in each SOA scheme affects the observed biases. Our analysis of the model performance of each scheme also provides the most suitable approach in simulating SOA in a typical urban environment. Comparisons of the simulated versus observed OA concentrations show that model biases range from −72% to +118%, with considerable variability among different schemes and seasons. We find that the inclusion of semi/intermediate volatile precursors, in addition to the traditional precursors, and chemical aging (functionalization) are important factors to simulate surface SOA concentrations in Seoul. However, a comparison of observed and simulated SOA/∆CO enhancement ratios suggests that most schemes underpredict SOA aging in upper levels in the boundary layer. We also find that the simplified SOA scheme can reproduce observed OA but often shows overestimation in surface air, indicating that uncertainties exist in bottom‐up emissions and precursor parameterization in Seoul. Plain Language Summary: We compare four different modeling approaches for simulating secondary organic aerosol (SOA) formation, accounting for a significant fraction of total fine particulate matter concentrations in Seoul, Korea. Using GEOS‐Chem, a chemical transport model, we find that current SOA schemes show large variabilities. Including an additional precursor species and further oxidation (i.e., chemical aging) of simulated SOA improves model performance. We also find that a simplified scheme with less computational cost can reproduce observed values but generally shows an overestimation in Seoul, indicating uncertainties in parameterization. Key Points: Model evaluation of simulated organic aerosols (OA) using different secondary organic aerosols (SOA) schemes in Seoul shows large variabilityThe inclusion of semi/intermediate volatile precursors and chemical aging are important factors in reducing model biasesThe simplified SOA scheme can reproduce observed OA, but uncertainties exist in precursor parameterization in Seoul [ABSTRACT FROM AUTHOR]

Abstract: While it is well known that combustion of ethanol as a biofuel will lead to enhanced emissions of methane, ethene (ethylene), acetaldehyde, formaldehyde, and oxides of nitrogen (primarily NO) when compared to gasoline alone, especially during cold starts or if catalytic converters are not operating properly, the impacts of increases in atmospheric ethene levels from combustion of fuels with higher ethanol content has not received much attention. Ethene is a well known and potent plant growth hormone and exposure to agricultural crops and natural vegetation results in yield reductions especially when combined with higher levels of PAN and ozone also expected from the increased use of ethanol/gasoline blends. We report here some baseline measurements of ethene obtained in 2002 in the southwestern and south central United States. These data indicate that current ethene background levels are less than 1 ppb. Anticipated increases in fuel ethanol content of E30 or greater is expected to lead to higher atmospheric levels of ethene on regional scales due to its atmospheric lifetime of 1.5–3 days. These background measurements are discussed in light of the potential enhancement of ethene levels expected from the anticipated increases in ethanol use as a renewable biofuel. [Copyright &y& Elsevier]

Laser printers are one of the common indoor equipment in schools, offices, and various other places. Laser printers have recently been identified as a potential source of indoor air pollution. This study examines the characteristics of ultrafine particles (UFPs, diameter <100 nm) and volatile organic compounds (VOCs) emitted from laser printers housed in a commercial printing center. The results indicated that apart from the printer type, the age of printers, and the number of pages printed, the characteristics of UFPs emitted from printers also depend on indoor ventilation conditions. It was found that at reduced ventilation rates of indoor air, there was a rise in the number concentration of UFPs in the printing center. Interestingly, the contribution of UFPs to the total number of submicrometer-sized particles was observed to be higher at a sampling point far away from the printer than the one in the immediate vicinity of the printer. Black carbon (BC) measurements showed a good correlation (rs = 0.82) with particles in the size range of 100-560 nm than those with diameters less than 100 nm (rs = 0.33 for 50-100 nm, and rs = -0.19 for 5.6-50 nm particles). Measurements of VOCs in the printing center showed high levels of m-, o-, and p-xylene, styrene, and ethylbenzenes during peak hours of printing. Although toluene was found in higher levels, its concentration decreased during peak hours compared to those during nonoperating hours of the printing center. [ABSTRACT FROM AUTHOR]

We use recent aircraft measurements of a comprehensive suite of anthropogenic halocarbons, carbon monoxide (CO), and related tracers to place new constraints on North American halocarbon emissions and quantify their global warming potential. Using a chemical transport model (GEOS-Chem) we find that the ensemble of observations are consistent with our prior best estimate of the U.S. anthropogenic CO source, but suggest a 30% underestimate of Mexican emissions. We develop an optimized CO emission inventory on this basis and quantify halocarbon emissions from their measured enhancements relative to CO. Emissions continue for many compounds restricted under the Montreal Protocol, and we show that halocarbons make up an important fraction of the total greenhouse gas source for both countries: our best estimate is 9% (uncertainty range 6-12%) and 32% (21-52%) of equivalent CO2 emissions for the U.S. and Mexico, respectively, on a 20 year time scale. Performance of bottom-up emission inventories is variable, with underestimates for some compounds and overestimates for others. Ongoing methylchloroform emissions are significant in the U.S. (2.8 Gg/y in 2004-2006), in contrast to bottom-up estimates (<0.05 Gg), with implications for tropospheric OH calculations. Mexican methylchloroform emissions are minor. [ABSTRACT FROM AUTHOR]

Various brands and types of cigarettes were purchased at retail locations in southern California. Volatile gas samples were analyzed using multicolumn/multidetector gas chromatography. Results showed methyl chloride (CH3Cl) levels as much as four orders of magnitude higher than typical urban levels, about 30-500 ppmv (1.5-5.3 mg/cigarette), compared with about 500 pptv in urban air. The concentration of CH3Cl correlated well with the levels of both CO (r 2 = 0.63) and CO2 (r 2 = 0.77), showing the link between CH3Cl and combustion. In some brands, CH3Cl levels were well above the U.S. Environmental Protection Agency's maximum exposure limit of 200 ppmv. Light branded cigarettes tended to have higher CH3Cl levels than the heavier and filtered brands, possibly showing the dependence of cigarette packing on CH3Cl production. In addition, CH3Cl emitted from cigarette smoke may prove to be an important anthropogenic source of CH3Cl in the United States, at about 5%. [ABSTRACT FROM AUTHOR]

We present data collected from a number of snow-covered environments including two polar locations (Summit, Greenland and the South Pole) and two mid-latitude regions (a remote site in northern Michigan, and Niwot Ridge, Colorado). At each site, concentrations of and were enhanced within the interstitial air near the snow surface, compared to levels in boundary layer air. Fluxes of from surface snow to the atmosphere were observed at each site except Niwot Ridge, where appeared to have a sink. The mid-latitude sites showed significant emissions of , mostly originating at the ground surface and traveling up through the snow, while at the polar locations emissions from firn air were relatively small. In general, methyl halide mixing ratios in firn air were significantly greater at Summit than at the South Pole, with Summit showing a strong diurnal cycle in the production of alkyl halides that was well correlated with actinic radiation and firn temperature. We suggest that the most likely route to alkyl halide formation is through an acid catalyzed nucleophilic substitution of an alcohol type function by a halide, both of which should be preferentially segregated to the quasi-liquid layer at the surface of the snow grains. A series of experiments using a snow-filled quartz chamber irradiated by natural sunlight allowed estimation of emission trends that were hard to measure in the natural snowpack. These static chamber experiments confirmed significant production of the primary alkyl halides, following the order . Our observations at all four locations, including polar and mid-latitude sites, imply that alkyl halide production may be associated with all surface snows. [Copyright &y& Elsevier]

Abstract: We report selected carbon species emission indices (EIs) for a Rolls Royce RB211-535-E4 turbofan engine that were acquired during the NASA EXperiment to Characterize Aircraft Volatile Aerosol and Trace-species Emissions (EXCAVATE). Conducted during winter 2002, the mission focused upon characterizing the exhaust constituents of the NASA Boeing 757 aircraft during ground-based operation. Carbon species concentrations were determined by chromatographic analyses of whole air samples collected 10m behind the engine exit plane as engine power was varied from ground idle to about 60% of maximum rated thrust. Ambient air samples were also collected and analyzed to facilitate correction of calculated EIs for background concentrations. Results are consistent with previous observations and indicate that, on a relative basis, turbine engines emit considerable amounts of light hydrocarbon species at idle, but significantly lesser amounts at higher engine powers. [Copyright &y& Elsevier]

Since 2012, studies in mice, rats, and humans have suggested that abnormalities in purinergic signaling may be a final common pathway for many genetic and environmental causes of autism spectrum disorder (ASD). The current study in mice was conducted to characterize the bioenergetic, metabolomic, breathomic, and behavioral features of acute hyperpurinergia triggered by systemic injection of the purinergic agonist and danger signal, extracellular ATP (eATP). Responses were studied in C57BL/6J mice in the maternal immune activation (MIA) model and controls. Basal metabolic rates and locomotor activity were measured in CLAMS cages. Plasma metabolomics measured 401 metabolites. Breathomics measured 98 volatile organic compounds. Intraperitoneal eATP dropped basal metabolic rate measured by whole body oxygen consumption by 74% ± 6% (mean ± SEM) and rectal temperature by 6.2˚ ± 0.3˚C in 30 minutes. Over 200 metabolites from 37 different biochemical pathways where changed. Breathomics showed an increase in exhaled carbon monoxide, dimethylsulfide, and isoprene. Metabolomics revealed an acute increase in lactate, citrate, purines, urea, dopamine, eicosanoids, microbiome metabolites, oxidized glutathione, thiamine, niacinamide, and pyridoxic acid, and decreased folate-methylation-1-carbon intermediates, amino acids, short and medium chain acyl-carnitines, phospholipids, ceramides, sphingomyelins, cholesterol, bile acids, and vitamin D similar to some children with ASD. MIA animals were hypersensitive to postnatal exposure to eATP or poly(IC), which produced a rebound increase in body temperature that lasted several weeks before returning to baseline. Acute hyperpurinergia produced metabolic and behavioral changes in mice. The behaviors and metabolic changes produced by ATP injection were associated with mitochondrial functional changes that were profound but reversible. [ABSTRACT FROM AUTHOR]

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr -1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr -1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr -1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr -1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr -1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr -1 , range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30 ∘ N) compared to mid-latitudes (∼ 30 %, 30–60 ∘ N) and high northern latitudes (∼ 4 %, 60–90 ∘ N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr -1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4 yr -1 by 8 Tg CH4 yr -1 , respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET- CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning. The data presented here can be downloaded from 10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from the Global Carbon Project. [ABSTRACT FROM AUTHOR]

Organic nitrates (RONO2) are an important NOx sink. In warm, rural environments dominated by biogenic emissions, nocturnal NO3‐initiated production of RONO2 is competitive with daytime OH‐initiated RONO2 production. However, in urban areas, OH‐initiated production of RONO2 has been assumed dominant and NO3‐initiated production considered negligible. We show evidence for nighttime RONO2 production similar in magnitude to daytime production during three aircraft campaigns in chemically distinct summertime environments: Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) in the rural Southeastern United States, Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ) in the Colorado Front Range, and Korea‐United States Air Quality Study (KORUS‐AQ) around the megacity of Seoul. During each campaign, morning observations show RONO2 enhancements at constant, near‐background Ox (≡ O3+NO2) concentrations, indicating that the RONO2 are from a non‐photochemical source, whereas afternoon observations show a strong correlation between RONO2 and Ox resulting from photochemical production. We show that there are sufficient precursors for nighttime RONO2 formation during all three campaigns. This evidence impacts our understanding of nighttime NOx chemistry. Plain Language Summary: Nitrogen oxides are pollutants emitted during combustion which are involved in ozone and secondary aerosol production. One way in which nitrogen oxides are removed from the atmosphere is via chemistry that converts them to organic nitrates. This conversion of nitrogen oxides to organic nitrates has been thought to occur primarily during the day when the chemistry is driven by sunlight. Here we show evidence that nighttime processes generate similar quantities of organic nitrates to those produced by sunlight‐driven processes. Key Points: We show evidence for nocturnal production of organic nitrates similar in magnitude to daytime photochemical productionSignificant nocturnal production of organic nitrates observed from three aircraft campaigns in distinct environmentsNighttime production of organic nitrates impacts our understanding of the nighttime lifetime and fate of NOx [ABSTRACT FROM AUTHOR]

The Community Earth System Model version 2 (CESM2) includes a detailed representation of chemistry throughout the atmosphere in the Community Atmosphere Model with chemistry and Whole Atmosphere Community Climate Model configurations. These model configurations use the Model for Ozone and Related chemical Tracers (MOZART) family of chemical mechanisms, covering the troposphere, stratosphere, mesosphere, and lower thermosphere. The new MOZART tropospheric chemistry scheme (T1) has a number of updates over the previous version (MOZART‐4) in CESM, including improvements to the oxidation of isoprene and terpenes, organic nitrate speciation, and aromatic speciation and oxidation and thus improved representation of ozone and secondary organic aerosol precursors. An evaluation of the present‐day simulations of CESM2 being provided for Climate Model Intercomparison Project round 6 (CMIP6) is presented. These simulations, using the anthropogenic and biomass burning emissions from the inventories specified for CMIP6, as well as online calculation of emissions of biogenic compounds, lightning NO, dust, and sea salt, indicate an underestimate of anthropogenic emissions of a variety of compounds, including carbon monoxide and hydrocarbons. The simulation of surface ozone in the southeast United States is improved over previous model versions, largely due to the improved representation of reactive nitrogen and organic nitrate compounds resulting in a lower ozone production rate than in CESM1 but still overestimates observations in summer. The simulation of tropospheric ozone agrees well with ozonesonde observations in many parts of the globe. The comparison of NOx and PAN to aircraft observations indicates the model simulates the nitrogen budget well. Plain Language Summary: The set of chemical reactions for tropospheric chemistry used in the Community Earth System Model version 2 (CESM2) has been updated significantly over CESM1 in the Community Atmosphere Model with chemistry (CAM‐chem) and Whole Atmosphere Community Climate Model (WACCM) configurations. The emissions used for the CESM2 simulations are documented here, with anthropogenic and biomass burning emissions based on the specified inventories for Climate Model Intercomparison Project 6 (CMIP6), and emissions of biogenic compounds, lightning NO, dust, and sea salt are calculated online and dependent on the simulated meteorology. Evaluation of the CAM‐chem and WACCM configurations of CESM2 with observations indicate an underestimate of anthropogenic emissions of a variety of compounds, including carbon monoxide and hydrocarbons. The updated chemistry leads to an improvement in the simulation of tropospheric ozone. Key Points: This paper fully documents the significant updates to the chemistry mechanisms in version 2 of the Community Earth System ModelThe new tropospheric chemistry scheme improves representation of isoprene oxidation as well as other ozone precursors over earlier versionsThe simulation of tropospheric ozone is improved in comparison to observations [ABSTRACT FROM AUTHOR]

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). Assessing the relative importance of CH4 in comparison to CO2 is complicated by its shorter atmospheric lifetime, stronger warming potential, and atmospheric growth rate variations over the past decade, the causes of which are still debated. Two major difficulties in reducing uncertainties arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (top-down approach) to be 572 Tg CH4 yr−1 (range 538–593, corresponding to the minimum and maximum estimates of the ensemble), of which 357 Tg CH4 yr−1 or ~ 60 % are attributed to anthropogenic sources (range 50–65 %). This total emission is 27 Tg CH4 yr−1 larger than the value estimated for the period 2000–2009 and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for the period 2003–2012 (Saunois et al. 2016). Since 2012, global CH4 emissions have been tracking the carbon intensive scenarios developed by the Intergovernmental Panel on Climate Change (Gidden et al., 2019). Bottom-up methods suggest larger global emissions (737 Tg CH4 yr−1, range 583–880) than top-down inversion methods, mostly because of larger estimated natural emissions from sources such as natural wetlands, other inland water systems, and geological sources. However the strength of the atmospheric constraints on the top-down budget, suggest that these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric-based emissions indicates a predominance of tropical emissions (~ 65 % of the global budget, < 30° N) compared to mid (~ 30 %, 30° N–60° N) and high northern latitudes (~ 4 %, 60° N–90° N). Our analyses suggest that uncertainties associated with estimates of anthropogenic emissions are smaller than those of natural sources, with top-down inversions yielding larger uncertainties than bottom-up inventories and models. The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some global source estimates are smaller compared to the previously published budgets (Saunois et al. 2016; Kirschke et al. 2013), particularly for vegetated wetland emissions that are lower by about 35 Tg CH4 yr−1 due to efforts to partition vegetated wetlands and inland waters. Emissions from geological sources are also found to be smaller by 7 Tg CH4 yr−1, and wild animals by 8 Tg CH4 yr−1. However the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of freshwater emissions resulting from recent research and the integration of emissions from estuaries. Priorities for improving the methane budget include: i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; ii) further development of process-based models for inland-water emissions; iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements and urban monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; iv) improvements of transport models and the representation of photochemical sinks in top-down inversions, and v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane. [ABSTRACT FROM AUTHOR]

Abstract Alkyl nitrates (RONO 2) are important reservoirs of nitrogen oxides and play key roles in the tropospheric chemistry. Two phases of intensive campaigns were conducted during February–April and June–July of 2017 at a rural coastal site and in open oil fields of the Yellow River Delta region, northern China. C 1 –C 5 alkyl nitrates showed higher concentration levels in summer than in winter-spring (p < 0.01), whilst their parent hydrocarbons showed an opposite seasonal variation pattern. The C 3 –C 5 RONO 2 levels in the oil fields were significantly higher than those in the ambient rural air. Alkyl nitrates showed well-defined diurnal variations, elucidating the effects of in-situ photochemical production and regional transport of aged polluted plumes. Backward trajectory analysis and fire maps revealed the significant contribution of biomass burning to the observed alkyl nitrates and hydrocarbons. A simplified sequential reaction model and an observation-based chemical box model were deployed to diagnose the formation mechanisms of C 1 –C 5 RONO 2. The C 3 –C 5 RONO 2 were mainly produced from the photochemical oxidation of their parent hydrocarbons (i.e., C 3 –C 5 alkanes), whilst C 1 –C 2 RONO 2 compounds have additional sources. In addition to parent hydrocarbons, longer alkanes with >4 carbon atoms were also important precursors of alkyl nitrates in the oil fields. This study demonstrates the significant effects of oil field emissions and biomass burning on the volatile organic compounds and alkyl nitrate formation, and provides scientific support for the formulation of control strategies against photochemical air pollution in the Yellow River Delta region. Graphical abstract Unlabelled Image Highlights • The tempo-spatial variations of C 1 -C 5 alkyl nitrates and parent hydrocarbons were examined in the Yellow River Delta. • Oil field emissions and biomass burning are important sources of hydrocarbons and alkyl nitrates in this region. • Besides parent hydrocarbons, longer alkanes are important precursors of alkyl nitrates in oil fields. [ABSTRACT FROM AUTHOR]

Both the Tiptop and Ruth Mullins coal fires, Kentucky, were reinvestigated in 2009 and 2010. The Tiptop fire was not as active in 2009 and may have been on the path to burning out at the time of the 2009 visit. The Ruth Mullins coal mine fire, Perry County, Kentucky, has been the subject of several field investigations, including November 2009–February 2010 investigations in which we measured gas emissions, collected minerals and tars, and characterized the nature of the fire. Vents exhibiting the greatest gas flux (>100,000 mg/s/m 2 ) are those with the largest amount of condensate minerals and tars. Vents with moderate gas flux (10,000–100,000 mg/s/m 2 ) are less likely to contain condensate minerals, but are collocated with tars, and vents with the lowest flux (<10,000 mg/s/m 2 ) generally lack both minerals and tars. Aliphatic hydrocarbons present in the gases include C1-C9 compounds, and aromatics include BTEX compounds. Diffuse-CO 2 emissions are concentrated along the fracture zones overlying abandoned mine works. The area of peak diffuse flux corresponds to the trend of the collapsed portal that forms vent 5. The greatest vent emissions were also recorded at vent 5. The snow-melt zone mapped in January 2010 overlies the areas of peak diffuse-CO 2 emissions measured in November; together they delineate the zone of active combustion. Comparison of greenhouse gas emissions from the two sources shows that vent emissions exceed diffuse emissions. The highly fractured, quartz-cemented roof rock funnels the majority of emissions toward the vents. Significant decreases are seen in estimates of yearly greenhouse emissions based on data gathered from November 2009 to February 2010, with estimates from November significantly exceeding any previously published estimates. For example, September 2009 estimates from vent 3 alone indicated that 19 ± 7.5 T CO 2 /yr were emitted while the November 2009 estimates were 1800 ± 690 T/yr. Barometric pressure was lower in November than September. This implies that there are many factors influencing the seasonal variations in fire emissions and that more frequent monitoring will be necessary to derive accurate estimates of coal fires' contribution to the carbon budget. [ABSTRACT FROM AUTHOR]

Alkyl nitrates (RONO 2 ) are an important class of nitrogen oxides reservoirs in the atmosphere and play a key role in tropospheric photochemistry. Despite the increasing concern for photochemical air pollution over China, the knowledge of characteristics and formation mechanisms of alkyl nitrates in this region is limited. We analyzed C 1 -C 5 alkyl nitrates measured in Beijing at a polluted urban site in summer 2008 and at a downwind rural site in summers of both 2005 and 2008. Although the abundances of NO x and hydrocarbons were much lower at the rural site, the mixing ratios of RONO 2 were comparable between both sites, emphasizing the regional nature of alkyl nitrate pollution. Regional transport of urban plumes governed the elevated RONO 2 levels at the rural site. The concentrations of C 1 -C 2 RONO 2 were significantly higher at the rural site in 2008 compared to 2005 despite a decline in NO x and anthropogenic VOCs, mainly owing to enhanced contributions from biogenic VOCs. The photochemical formation regimes of RONO 2 were evaluated by both a simplified sequential reaction model and a detailed master chemical mechanism box model. The observed C 4 -C 5 RONO 2 levels can be well explained by the photochemical degradation of n -butane and n -pentane, while the sources of C 1 -C 3 RONO 2 were rather complex. In addition to the C 1 -C 3 alkanes, biogenic VOCs and reactive aromatics were also important precursors of methyl nitrate, and alkenes and long-chain alkanes contributed to the formation of C 2 -C 3 RONO 2 . This study provides insights into the spatial distribution, inter-annual variation and photochemical formation mechanisms of alkyl nitrate pollution over the Beijing area. [ABSTRACT FROM AUTHOR]

This work reports the first ground-based atmospheric measurements of 26 halocarbons in Singapore, an urban-industrial city-state in Southeast (SE) Asia. A total of 166 whole air canister samples collected during two intensive 7 Southeast Asian Studies (7SEAS) campaigns (August–October 2011 and 2012) were analyzed for C 1 -C 2 halocarbons using gas chromatography-electron capture/mass spectrometric detection. The halocarbon dataset was supplemented with measurements of selected non-methane hydrocarbons (NMHCs), C 1 -C 5 alkyl nitrates, sulfur gases and carbon monoxide to better understand sources and atmospheric processes. The median observed atmospheric mixing ratios of CFCs, halons, CCl 4 and CH 3 CCl 3 were close to global tropospheric background levels, with enhancements in the 1–17% range. This provided the first measurement evidence from SE Asia of the effectiveness of Montreal Protocol and related national-scale regulations instituted in the 1990s to phase-out ozone depleting substances (ODS). First- and second-generation CFC replacements (HCFCs and HFCs) dominated the atmospheric halocarbon burden with HFC-134a, HCFC-22 and HCFC-141b exhibiting enhancements of 39–67%. By combining near-source measurements in Indonesia with receptor data in Singapore, regionally transported peat-forest burning smoke was found to impact levels of several NMHCs (ethane, ethyne, benzene, and propane) and short-lived halocarbons (CH 3 I, CH 3 Cl, and CH 3 Br) in a subset of the receptor samples. The strong signatures of these species near peat-forest fires were potentially affected by atmospheric dilution/mixing during transport and by mixing with substantial urban/regional backgrounds at the receptor. Quantitative source apportionment was carried out using positive matrix factorization (PMF), which identified industrial emissions related to refrigeration, foam blowing, and solvent use in chemical, pharmaceutical and electronics industries as the major source of halocarbons (34%) in Singapore. This was followed by marine and terrestrial biogenic activity (28%), residual levels of ODS from pre-Montreal Protocol operations (16%), seasonal incidences of peat-forest smoke (13%), and fumigation related to quarantine and pre-shipment (QPS) applications (7%). [ABSTRACT FROM AUTHOR]

The Lotts Creek coal mine fire is burning in abandoned works of the Pennsylvanian Hazard No. 9 coal, Perry County, Kentucky. Over the few months separating sampling trips, the fire showed a definite migration to the south. Several vents sampled on the first trip were extinct on the second trip. The flux of major gases varies from 1100 to 440,000 mg/s/m 2 CO 2 and < 100 to 12,000 mg/s/m 2 CO, with the gas temperature being one of the principal drivers of the emissions variations; the higher the temperature, the more CO 2 produced. Mercury, also showing wide variation, from 45 to 740 ng/s/m 2 , could not be measured at all vents due to temperature limitations inherent in the instrument. In addition to CO 2 , CO, and Hg, a number of gases among the volatile aliphatic and volatile aromatic compounds are emitted in potentially dangerous amounts. [ABSTRACT FROM AUTHOR]

Oil and natural gas operations have continued to expand and move closer to densely populated areas, contributing to growing public concerns regarding exposure to hazardous air pollutants. During the Barnett Shale Coordinated Campaign in October, 2013, ground-based whole air samples collected downwind of oil and gas sites revealed enhancements in several potentially toxic volatile organic compounds (VOCs) when compared to background values. Molar emissions ratios relative to methane were determined for hexane, benzene, toluene, ethylbenzene, and xylene (BTEX compounds). Using methane leak rates measured from the Picarro mobile flux plane (MFP) system and a Barnett Shale regional methane emissions inventory, the rates of emission of these toxic gases were calculated. Benzene emissions ranged between 51 ± 4 and 60 ± 4 kg h-1. Hexane, the most abundantly emitted pollutant, ranged from 642 ± 45 to 1070 ± 340 kg h-1. While observed hydrocarbon enhancements fall below federal workplace standards, results may indicate a link between emissions from oil and natural gas operations and concerns about exposure to hazardous air pollutants. The larger public health risks associated with the production and distribution of natural gas are of particular importance and warrant further investigation, particularly as the use of natural gas increases in the United States and internationally. [ABSTRACT FROM AUTHOR]

Plants play a crucial role in global carbon biogeochemical cycling and natural terrestrial carbon sinks. Dynamic changes in plant-related carbon cycling processes under changing climate and atmospheric compositions are hot scientific issues concerning carbon neutrality. Ozone, as a damaging oxidant, shows a rising trend near the ground where plants grow, directly and indirectly impacting forests and other types of vegetation. This review focuses on the effects of elevated atmospheric ozone levels on plant-related carbon cycling processes, including carbon dioxide (CO 2) assimilation, carbon allocation to roots, volatile emissions, soil carbon sequestration and litter decomposition. Based on previous studies, we propose that field observations, especially in situ long-term observations under natural growing conditions in well-designed networks with a better representation, are needed to deeply understand the effects of elevated ozone on plants. Apart from an overwhelming concern about the influence of ozone on crop yields, studies on the effects of elevated ozone on forests, especially tropical and subtropical forests, should be strengthened in the future. Meanwhile, the interactions between ozone and plants should be considered in understanding plants' feedback to oxidants through emissions of volatiles and other trace gases. Moreover, geochemical techniques such as carbon isotopes and molecular markers, along with big data and artificial intelligence approaches, can be extensively used to decode and constrain the ozone-plant relationships, such as those between net primary productivity and ozone. • The effects of elevated ozone on plant-related carbon cycling processes are summarized. • In situ long-term observations under natural growing conditions are needed. • Feedbacks of plants to atmospheric oxidants should be considered in ozone-plant interactions. [ABSTRACT FROM AUTHOR]

National-scale emissions of carbon tetrachloride (CCl4) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration's flask air sampling network. We estimate an annual average US emission of 4.0 (2.0-6.5) Gg CCl4 y-1 during 2008-2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y-1) but only 8% (3-22%) of global CCl4 emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl4 emission during 2008-2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl4 throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl4 sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach). [ABSTRACT FROM AUTHOR]

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (T-D, exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories, and data-driven approaches (B-U, including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by T-D inversions at 558 & Tg & CH4 & yr-1 (range [540-568]). About 60 & % of global emissions are anthropogenic (range [50-65 & %]). B-U approaches suggest larger global emissions (736 & Tg & CH4 & yr-1 [596-884]) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the T-D budget, it is likely that some of the individual emissions reported by the B-U approaches are overestimated, leading to too large global emissions. Latitudinal data from T-D emissions indicate a predominance of tropical emissions (~64 & % of the global budget, < & 30° & N) as compared to mid (~32 & %, 30° & N-60° & N) and high northern latitudes (~ & 4 & %, 60° & N-90° & N). T-D inversions consistently infer lower emissions in China (~58 & Tg & CH4 & yr-1 [51-72], -14 & %) and higher emissions in Africa (86 & Tg & CH4 & yr-1 [73-108], +19 & %) than B-U values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for T-D inversions than for B-U inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute for 30-40 & % on the estimated range for wetland emissions. Other priorities for improving the methane budget include: i) the development of process-based models for inland-water emissions, ii) the intensification of methane observations at local scale (flux measurements) to constrain B-U land surface models, and at regional scale (surface networks and satellites) to constrain T-D inversions, iii) improvements in the estimation of atmospheric loss by OH, and iv) improvements of the transport models integrated in T-D inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (doi:10.3334/CDIAC/Global_Methane_Budget_2016). [ABSTRACT FROM AUTHOR]

Particulate air pollution is a health concern. This study determines the microscopic make-up of different varieties of sand particles collected at a sand dune site in Badr, Saudi Arabia in 2012. Three categories of sand were studied: black sand, white sand, and volcanic sand. The study used multiple high resolution electron microscopies to study the morphologies, emission source types, size, and elemental composition of the particles, and to evaluate the presence of surface "coatings or contaminants" deposited or transported by the black sand particles. White sand was comprised of natural coarse particles linked to wind-blown releases from crustal surfaces, weathering of igneous/metamorphic rock sources, and volcanic activities. Black sand particles exhibited different morphologies and microstructures (surface roughness) compared with the white sand and volcanic sand. Morphological Scanning Electron Microscopy (SEM) and Laser Scanning Microscopy (LSM) analyses revealed that the black sand contained fine and ultrafine particles (50 to 500 nm ranges) and was strongly magnetic, indicating the mineral magnetite or elemental iron. Aqueous extracts of black sands were acidic (pH = 5.0). Fe, C, O, Ti, Si, V, and S dominated the composition of black sand. Results suggest that carbon and other contaminant fine particles were produced by fossil-fuel combustion and industrial emissions in heavily industrialized areas of Haifa and Yanbu, and transported as cloud condensation nuclei to Douf Mountain. The suite of techniques used in this study has yielded an in-depth characterization of sand particles. Such information will be needed in future environmental, toxicological, epidemiological, and source apportionment studies. [ABSTRACT FROM AUTHOR]

Vehicular emission is one of the important anthropogenic pollution sources for volatile organic compounds (VOCs). Four characterization campaigns were conducted at a representative urban roadside environment in Hong Kong between May 2011 and February 2012. Carbon monoxide (CO) and VOCs including methane (CH 4 ), non-methane hydrocarbons (NMHCs), halocarbons, and alkyl nitrates were quantified. Both mixing ratios and compositions of the target VOCs show ignorable seasonal variations. Except CO, liquefied petroleum gas (LPG) tracers of propane, i -butane and n -butane are the three most abundant VOCs, which increased significantly as compared with the data measured at the same location in 2003. Meanwhile, the mixing ratios of diesel- and gasoline tracers such as ethyne, alkenes, aromatics, halogenated, and nitrated hydrocarbons decreased by at least of 37%. The application of advanced multivariate receptor modeling technique of positive matrix factorization (PMF) evidenced that the LPG fuel consumption is the largest pollution source, accounting for 60 ± 5% of the total quantified VOCs at the roadside location. The sum of ozone formation potential (OFP) for the target VOCs was 300.9 μg-O 3 m −3 , which was 47% lower than the value of 567.3 μg-O 3 m −3 measured in 2003. The utilization of LPG as fuel in public transport (i.e., taxis and mini-buses) contributed 51% of the sum of OFP, significantly higher than the contributions from gasoline- (16%) and diesel-fueled (12%) engine emissions. Our results demonstrated the effectiveness of the switch from diesel to LPG-fueled engine for taxis and mini-buses implemented by the Hong Kong Special Administrative Region (HKSAR) Government between the recent ten years, in additional to the execution of substitution to LPG-fueled engine and restrictions of the vehicular emissions in compliance with the updated European emission standards. [ABSTRACT FROM AUTHOR]

Sulfuric acid (H2SO4), formed from oxidation of sulfur dioxide (SO2) emitted during fossil fuel combustion, is a major precursor of new airborne particles, which have well-documented detrimental effects on health, air quality, and climate. Another precursor is methanesulfonic acid (MSA), produced simultaneously with SO2 during the atmospheric oxidation of organosulfur compounds (OSCs), such as dimethyl sulfide. In the present work, a multidisciplinary approach is used to examine how contributions of H2SO4 and MSA to particle formation will change in a large coastal urban area as anthropogenic fossil fuel emissions of SO2 decline. The 3-dimensional University of California Irvine-California Institute of Technology airshed model is used to compare atmospheric concentrations of gas phase MSA, H2SO4, and SO2 under current emissions of fossil fuel-associated SO2 and a best-case futuristic scenario with zero fossil fuel sulfur emissions. Model additions include results from (i) quantum chemical calculations that clarify the previously uncertain gas phase mechanism of formation of MSA and (ii)a combination of published and experimental estimates of OSC emissions, such as those from marine, agricultural, and urban processes, which include pet waste and human breath. Results show that in the zero anthropogenic SO2 emissions case, particle formation potential from H2SO4 will drop by about two orders of magnitude compared with the current situation. However, particles will continue to be generated from the oxidation of natural and anthropogenic sources of OSCs, with contributions from MSA and H2SO4 of a similar order of magnitude. This could be particularly important in agricultural areas where there are significant sources of OSCs. [ABSTRACT FROM AUTHOR]

Inhaled corticosteroids (ICS) and β2-agonists are the primary pharmacotherapies of asthma management. However, suboptimal medication compliance is common in asthmatics and is associated with increased morbidity. We hypothesized that exhaled breath measurements of the aerosol used in the inhaled medications might prove useful as surrogate marker for asthma medication compliance. To explore this, 10 healthy controls were recruited and randomly assigned to ICS (Flovent HFA) or short acting bronchodilators (Proventil HFA). Both inhalers contain HFA-134a as aerosol propellant. Exhaled breath sampling and pulmonary function tests were performed prior to the inhaler medication dispersion, immediately after inhalation, then at 2, 4, 6, 8, 24, and 48 hours postadministration. At baseline, mean (SD) levels of HFA-134a in the breath were 252 (156) pptv. Immediately after inhalation, HFA-134a breath levels increased to 300 × 106 pptv and were still well above ambient levels 24 hours postadministration. The calculated ratio of forced expiratory volume in 1 second over forced vital capacity did not change over time following inhaler administration. This study demonstrates, for the first time, that breath HFA-134a levels can be used to assess inhaler medication compliance. It may also be used to evaluate how effectively the medicine is delivered. [ABSTRACT FROM AUTHOR]

A growing dependence on natural gas for energy may exacerbate emissions of the greenhouse gas methane (CH4). Identifying fingerprints of these emissions is critical to our understanding of potential impacts. Here, we compare stable isotopic and alkane ratio tracers of natural gas, agricultural, and urban CH4 sources in the Barnett Shale hydraulic fracturing region near Fort Worth, Texas. Thermogenic and biogenic sources were compositionally distinct, and emissions from oil wells were enriched in alkanes and isotopically depleted relative to natural gas wells. Emissions from natural gas production varied in δ13C and alkane ratio composition, with δD-CH4 representing the most consistent tracer of natural gas sources. We integrated our data into a bottom-up inventory of CH4 for the region, resulting in an inventory of ethane (C2H6) sources for comparison to top-down estimates of CH4 and C2H6 emissions. Methane emissions in the Barnett are a complex mixture of urban, agricultural, and fossil fuel sources, which makes source apportionment challenging. For example, spatial heterogeneity in gas composition and high C2H6/CH4 ratios in emissions from conventional oil production add uncertainty to top-down models of source apportionment. Future top-down studies may benefit from the addition of δD-CH4 to distinguish thermogenic and biogenic sources. [ABSTRACT FROM AUTHOR]

It is challenging to reduce ground-level ozone (O3) pollution at a given locale, due in part to the contributions of both local and distant sources. We present direct evidence that the increasing regional effects have negated local control efforts for O3 pollution in Hong Kong over the past decade, by analyzing the daily maximum 8 h average O3 and Ox (=O3+NO2) concentrations observed during the high O3 season (September-November) at Air Quality Monitoring Stations. The locally produced Ox showed a statistically significant decreasing trend over 2002-2013 in Hong Kong. Analysis by an observation-based model confirms this decline in in situ Ox production, which is attributable to a reduction in aromatic hydrocarbons. However, the regional background Ox transported into Hong Kong has increased more significantly during the same period, reflecting contributions from southern/eastern China. The combined result is a rise in O3 and a nondecrease in Ox. This study highlights the urgent need for close cross-boundary cooperation to mitigate the O3 problem in Hong Kong. China's air pollution control policy applies primarily to its large cities, with little attention to developing areas elsewhere. The experience of Hong Kong suggests that this control policy does not effectively address secondary pollution, and that a coordinated multiregional program is required. [ABSTRACT FROM AUTHOR]

The Arabian Peninsula experiences severe air pollution, the extent and sources of which are poorly documented. Each year in Saudi Arabia this situation is intensified during Hajj, the Holy Pilgrimage of Islam that draws millions of pilgrims to Mecca. An initial study of air quality in Mecca and surrounding holy sites during the 2012 Hajj (October 24-27) revealed strongly elevated levels of the combustion tracer carbon monoxide (CO, up to 57 ppmv) and volatile organic compounds (VOCs) along the pilgrimage route-especially in the tunnels of Mecca-that are a concern for human health. The most abundant VOC was the gasoline evaporation tracer i-pentane, which exceeded 1200 ppbv in the tunnels. Even though VOC concentrations were generally lower during a follow-up non-Hajj sampling period (April 2013), many were still comparable to other large cities suffering from poor air quality. Major VOC sources during the 2012 Hajj study included vehicular exhaust, gasoline evaporation, liquefied petroleum gas, and air conditioners. Of the measured compounds, reactive alkenes and CO showed the strongest potential to form ground-level ozone. Because the number of pilgrims is expected to increase in the future, we present emission reduction strategies to target both combustive and evaporative fossil fuel sources. [ABSTRACT FROM AUTHOR]