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Dry conditions associated with the El Niño–Southern Oscillation (ENSO) and a positive Indian Ocean Dipole (IOD) are known to have caused major fire pollution events and intense carbon emissions over a vast spatial expanse of Indonesia in October 2006 and 2015. During these two events, a substantial increase in the carbon monoxide (CO) mixing ratio was detected by in situ measurements at Lulin Atmospheric Background Station (LABS; 23.47∘ N 120.87∘ E; 2862 ma.s.l.) in Taiwan, which is the only background station in the subtropical western North Pacific region. Compared to the long-term October mean (2006–2021), CO was elevated by ∼ 47.2 ppb (parts per billion; 37.2 %) and ∼ 36.7 ppb (28.9 %) in October 2006 and 2015, respectively. This study delineates plausible pathways for the CO transport from Indonesia to LABS using Measurement of Pollution in the Troposphere (MOPITT) CO observations and Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) reanalysis products (winds and geopotential height – GpH). Two simultaneously occurring transport pathways were identified, namely (i) horizontal transport in the free troposphere and (ii) vertical transport through the Hadley circulation (HC). The GpH analysis of both events revealed the presence of a high-pressure anticyclone over the northern part of the South China Sea (SCS), which played an important role in the free-tropospheric horizontal transport of CO. In this scenario, CO in the free troposphere is transported on the western edge of the high-pressure system and then driven by subtropical westerlies to LABS. Simultaneously, uplifted CO over Indonesia can enter the HC and be transferred to subtropical locations such as LABS. The vertical cross section of the MOPITT CO and MERRA-2 vertical pressure velocity supported the transport of CO through the HC. Furthermore, the results revealed a distinct HC strength in two events (higher in 2006 compared to 2015) due to the different ENSO conditions. Overall, the present findings can provide some insights into understanding the regional transport of pollution over Southeast Asia and the role of climate conditions on transport pathways.

Airborne volatile organic compounds (VOCs) and semi-volatile organic compounds (SVOCs) are commonly quantitated by collecting the analytes on solid sorbent tubes or passive air samplers, followed by solvent extraction and instrumental analysis, or by grab bag/canister measurements. We report herein a user-friendly sampling method by breathing through polyurethane foam (PUF) face masks to collect airborne VOCs and SVOCs for chemical analysis. Specifically, dibasic esters, phthalate esters, polycyclic aromatic hydrocarbons, linalool, and nicotine trapped on PUF masks were quantitated by gas chromatography-mass spectrometry analysis as model VOCs and SVOCs. Results showed that the amount of these model VOCs and SVOCs trapped on PUF masks is proportional to the exposure duration. After cross-validation by parallel sampling using XAD-2 packed sorbent tubes, the method was used to quantitate VOCs and SVOCs in a variety of indoor and outdoor environments with varying air concentrations of analytes, temperature, humidity, and wind speed. Because air pollution is considered a major cause of many human diseases and premature deaths and the developed PUF mask sampling method showed high trapping efficiencies for both VOCs and SVOCs, it is believed that the developed sampling method will find wide application in assessing air pollution-associated disease risks with possible extension to more classes of VOCs and SVOCs when coupled with suitable instrumental detection methods.

Anthropogenic pollution, including primary compounds such as nitrogen oxides (NOx) and organics, but also secondary pollutants such as ozone, are a threat to sensitive mountain ecosystems, which are already under continued threat of diminished area, due to climate change. This study analyzes two days of volatile organic compound (VOC) concentrations, including a limited set of carbonyls, at the Lulin Atmospheric Background Station (LABS; 2,862 meters asl), which is a well-known remote sub-tropical site that receives long-range transported air masses from various clean and polluted origins. VOCs were sampled in a canister and analyzed by GC-MS/FID, while carbonyls were trapped on Supelco DNPH-coated cartridges and quantified by HPLC-UV. Routine LABS measurements of ozone, CO, and PM2.5 were also utilized; Copernicus Atmospheric Monitoring Service (CAMS) reanalysis NOx and HNO3 concentrations were further incorporated into an oxidant modeling analysis. In comparing the two sampling days, the first day was characterized by hazier conditions (~3 times higher PM2.5 concentrations) and 2-3 times higher VOC and CO concentrations and calculated OH reactivity values. Based on a HYSPLIT back-trajectory analysis, the first day was influenced by air that had a longer residence time at lower altitudes over South China, while the second day was characterized by higher level transport. Also influential at the site are subsidence events that bring drier air that can contain high ozone and NOy species. The measurement and reanalysis data were incorporated into a 0-dimensional modeling analysis (F0AM) of the gas-phase oxidation chemistry in order to further characterize the different air masses that influence this sensitive mountain area. While the first day also was simulated to have higher level of ozone production, the second day captured an afternoon spike in pollutants and ozone production that was likely driven by upslope mountain valley air sourced for lower altitudes in Taiwan. Thus, the oxidation potential in this environment is characterized by large swings driven by local upslope pollution, subsidence events, and long-range transported pollution from the Asian continent, which ultimately dictate the pollutant exposure for this sensitive ecosystem.

Atmospheric mercury (Hg) cycling is sensitive to climate-driven changes, but links with various teleconnections remain unestablished. Here, we revealed the El Niño-Southern Oscillation (ENSO) influence on gaseous elemental mercury (GEM) concentrations recorded at a background station in East Asia using the Hilbert-Huang transform (HHT). The timing and magnitude of GEM intrinsic variations were clearly distinguished by ensemble empirical mode decomposition (EEMD), revealing the amplitude of the GEM concentration interannual variability (IAV) is greater than that for diurnal and seasonal variability. We show that changes in the annual cycle of GEM were modulated by significant IAVs at time scales of 2-7 years, highlighted by a robust GEM IAV-ENSO relationship of the associated intrinsic mode functions. With confirmation that ENSO modulates the GEM annual cycle, we then found that weaker GEM annual cycles may have resulted from El Niño-accelerated Hg evasion from the ocean. Furthermore, the relationship between ENSO and GEM is sensitive to extreme events (i.e., 2015-2016 El Niño), resulting in perturbation of the long-term trend and atmospheric Hg cycling. Future climate change will likely increase the number of extreme El Niño events and, hence, could alter atmospheric Hg cycling and influence the effectiveness evaluation of the Minamata Convention on Mercury.

Photochemical ozone pollution is a serious air quality problem under weak synoptic conditions in many areas worldwide. Volatile organic compounds (VOCs) are largely responsible for ozone production in urban areas where NOx mixing ratios are high while usually not a limiting precursor to ozone. In this study, the Community Multiscale Air Quality model – Higher-order Direct Decoupled Method (CMAQ-HDDM) at an urban-scale resolution (1.0 km x 1.0 km) in conjunction with positive matrix factorization (PMF) was used to identify the dominant sources of highly sensitive VOC species to ozone formation in southern Taiwan, a complex region of coastal urban and industrial parks and inland mountainous areas. First-order, second-order and cross sensitivities of ozone concentrations to domain-wide (i.e. urban, suburban and rural) NOx and VOC emissions were determined for the study area. Negative (positive) first-order sensitivities to NOx emissions are dominant over urban (inland) areas, confirming ozone production sensitivity favors the VOC-limited regime (NOx-limited regime) in southern Taiwan. Furthermore, most of the urban areas also exhibited negative second-order sensitivity to NOx emissions, indicating a negative O3 convex response where the linear increase of O3 from decreasing NOx emissions was largely attenuated by the non-linear effects. Due to the solidly VOC-limited regime and the relative insensitivity of O3 production to increases or decreases of NOx emissions, this study pursued the VOC species that contributed the most to ozone formation. PMF analysis driven by VOCs resolved 8 factors including mixed industry (21 %), vehicle emissions (22 %), solvent usage (17 %), biogenic (12 %), plastic industry (10 %), aged air mass (7 %), motorcycle exhausts (7 %), and manufacturing industry (5 %). Furthermore, a composite index that quantitatively combined the CMAQ-HDDM sensitivity coefficient and PMF resolved factor contribution, was developed to identify the key VOC species that should be targeted for effective ozone abatement. Our results indicate that VOC control measures should target on (1) solvent usage for painting, coating and the printing industry, which emits abundant toluene and xylene, (2) gasoline fuel vehicle emissions of n-butane, isopentane, isobutane and n-pentane, and (3) ethylene and propylene emissions from the petrochemical industry.

Dry conditions associated with El Niño and a positive Indian Ocean Dipole (IOD) are known to have caused major fire pollution events and intense carbon emissions over a vast spatial expanse of Indonesia in October 2006 and 2015. During these two events, a substantial increase in carbon monoxide (CO) mixing ratio was detected by in-situ measurements at Lulin Atmospheric Background Station (LABS, 23.47° N 120.87° E, 2,862 m ASL) in Taiwan, the only background station in the subtropical western North Pacific region. Compared to the long-term October mean (2006–2021), CO was elevated by ~47.2 ppb (37.2 %) and ∼36.7 ppb (28.9 %) in October 2006 and 2015, respectively. In this study, plausible pathways for CO transport from Indonesia to LABS are delineated by using MOPITT CO observations and MERRA-2 reanalysis products (winds and geopotential height (GpH)). Two simultaneously occurring transport pathways were identified: (i) horizontal transport in the free troposphere and (ii) vertical transport through the Hadley circulation (HC). The GpH analysis of both events revealed the presence of a high-pressure anticyclone over the northern part of the South China Sea (SCS), which played an important role in the free tropospheric horizontal transport of CO. In this scenario, CO in the free troposphere is transported on the western edge of the high-pressure system and then driven by subtropical westerlies to LABS. Simultaneously, uplifted CO over Indonesia can enter the HC and transfer to subtropical locations such as LABS. The vertical cross-section of MOPITT CO and MERRA-2 vertical pressure velocity supported the transport of CO through the HC. Further, the results revealed a distinct HC strength in two events (higher in 2006 compared to 2015) due to the different El Niño conditions. Overall, the present findings can provide some insights into understanding the regional transport of pollution over Southeast Asia and the role of climate conditions on transport pathways.

In this work, we deployed a single particle aerosol mass spectrometer (SPAMS) at a suburban coastal site in Hong Kong from February 04 to April 17, 2013 to study individual oxalate particles and a monitor for aerosols and gases in ambient air (MARGA) to track the bulk oxalate concentrations in particle matter smaller than 2.5 μm in diameter (PM

INTRODUCTION Coronavirus disease 2019 (COVID-19) emerged in Wuhan, China in late 2019, and soon unfolded as a global outbreak accompanied by declarations of a public health emergency of international concern (PHEIC) and later a pandemic from the World Health Organization (WHO). COVID-19 has resulted in 2,626,321 confirmed cases and 181,938 reported deaths worldwide (as of 14 April 2020). The underlying virus, severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), is a highly contagious novel coronavirus that transmits as an aerosol and threatens people of all ages, from infant to geriatric, while those with cardiovascular disease are recognized as particularly susceptible to more severe symptoms from SARS-CoV-2 infection. WHO recommends using a mask to limit the COVID-19 outbreak; however, SARS-CoV-2 transmission models and its removal efficiency by wearing a mask remain unclear. Furthermore, differences in the field-specific definitions/terminologies related to transmission and mask usage tend to cause confusion and misunderstanding among both experts and the public.

Surgical masks have been worn by the public worldwide during the COVID-19 pandemic, yet hazardous chemicals in the petroleum-derived polymer layer of masks are currently ignored and unregulated. These organic compounds pose potential health risks to the mask wearer through dermal contact or inhalation. Here, we show that surgical masks from around the world are loaded with semivolatile and volatile organic compounds (VOCs), including alkanes, polycyclic aromatic hydrocarbons (PAHs), phthalate esters, and reactive carbonyls at ng to μg/mask levels. Naphthalene was the most abundant mask-borne PAH, accounting for over 80% of total PAH levels; acrolein, a mutagenic carbonyl, was detected in most of the mask samples, and di(2-ethylhexyl) phthalate, an androgen antagonist, was detected in one-third of the samples. Furthermore, there is large mask-to-mask variability of the residue VOCs, revealing the uneven quality of masks. We confirm that masks containing more residue VOCs lead to significantly higher exposure levels and associated disease risks to the wearer, which should warrant the attention of the general public and regulatory agencies. We find that heating the masks at 50 °C for as short as 60 min lowers the total VOC content by up to 80%, providing a simple method to limit our exposure to mask-borne VOCs.

This study aimed to develop a technique to chemically characterize odor issues in neighborhoods of designated industrial zones with pronounced emissions of volatile organic compounds (VOCs). Due to the elusive nature of odor plumes, speedy detection with sufficient sensitivity is required to capture the plumes. In this demonstration, proton-transfer-reaction mass spectrometry (PTR-MS) was used as the front-line detection tool in an industrial zone to guide sampling canisters for in-laboratory analysis of 106 VOCs by gas chromatography-mass spectrometry/flame ionization detector (GC-MS/FID). The fast but less accurate PTR-MS coupled with the slow but accurate GC-MS/FID method effectively eliminates the drawbacks of each instrument and fortifies the strength of both when combined. A 10-day PTR-MS field screening period was conducted to determine suitable trigger VOC species with exceedingly high mixing ratios that were likely the culprits of foul odors. Twenty canister samples were then collected, triggered by m/z 43, 61 (ethyl acetate, fragments, EA), m/z 73 (methyl ethyl ketone, MEK), or m/z 88 (morpholine) in all cases. Internal consistency was confirmed by the high correlation of critical species in the PTR-MS and trigger samples. Several long-lived halocarbons were exploited as the intrinsic internal reference for quality assurance. Oxygenated VOCs (OVOCs) accounted for 15%-75% of the total VOC mixing ratios in the triggered samples. However, EA and MEK, the most prominent OVOC species, did not appear to have common sources with morpholine, which presented with PTR-MS peaks incoherent with the other OVOCs. Nevertheless, these distinctive OVOC plumes were consistent with the multiple types of odor reported by the local residents. In contrast with the triggered sampling, random samples in the same industrial zone and roadside samples in a major metropolitan area were collected. The pronounced OVOC content in the triggered samples highlighted the advantage over random grab sampling to address odor issues.

Aerosol type plays a critical role in the relationship between aerosol optical depth (AOD) and particulate matter (PM) mass concentration. Here, we present a mathematical formulation of how PM...

Semi-volatile and intermediate-volatility organic compounds (SVOCs and IVOCs) from anthropogenic sources are likely to be important precursors of secondary organic aerosol (SOA) in urban airsheds, yet their treatment in most models is based on limited and obsolete data or completely missing. Additionally, gas-phase oxidation of organic precursors to form SOA is influenced by the presence of nitric oxide (NO), but this influence is poorly constrained in chemical transport models. In this work, we updated the organic aerosol model in the UCD/CIT (University of California at Davis/California Institute of Technology) chemical transport model to include (i) a semi-volatile and reactive treatment of primary organic aerosol (POA), (ii) emissions and SOA formation from IVOCs, (iii) the NOx influence on SOA formation, and (iv) SOA parameterizations for SVOCs and IVOCs that are corrected for vapor wall loss artifacts during chamber experiments. All updates were implemented in the statistical oxidation model (SOM) that simulates the oxidation chemistry, thermodynamics, and gas–particle partitioning of organic aerosol (OA). Model treatment of POA, SVOCs, and IVOCs was based on an interpretation of a comprehensive set of source measurements available up to the year 2016 and resolved broadly by source type. The NOx influence on SOA formation was calculated offline based on measured and modeled VOC:NOx ratios. Finally, the SOA formation from all organic precursors (including SVOCs and IVOCs) was modeled based on recently derived parameterizations that accounted for vapor wall loss artifacts in chamber experiments. The updated model was used to simulate a 2-week summer episode over southern California at a model resolution of 8 km. When combustion-related POA was treated as semi-volatile, modeled POA mass concentrations were reduced by 15 %–40 % in the urban areas in southern California but were still too high when compared against “hydrocarbon-like organic aerosol” factor measurements made at Riverside, CA, during the Study of Organic Aerosols at Riverside (SOAR-1) campaign of 2005. Treating all POA (except that from marine sources) to be semi-volatile, similar to diesel exhaust POA, resulted in a larger reduction in POA mass concentrations and allowed for a better model–measurement comparison at Riverside, but this scenario is unlikely to be realistic since this assumes that POA from sources such as road and construction dust are semi-volatile too. Model predictions suggested that both SVOCs (evaporated POA vapors) and IVOCs did not contribute as much as other anthropogenic precursors (e.g., alkanes, aromatics) to SOA mass concentrations in the urban areas (NOx-dependent. Accounting for the influence of NOx using the VOC:NOx ratios resulted in better predictions of OA mass concentrations in rural/remote environments but still underpredicted OA mass concentrations in urban environments. The updated model's performance against measurements combined with the results from the sensitivity simulations suggests that the OA mass concentrations in southern California are constrained within a factor of 2. Finally, simulations performed for the year 2035 showed that, despite reductions in VOC and NOx emissions in the future, SOA mass concentrations may be higher than in the year 2005, primarily from increased hydroxyl radical (OH) concentrations due to lower ambient NO2 concentrations.

Continental outflows from peninsular Southeast Asia and East Asia dominate the widespread dispersal of air pollutants over subtropical western North Pacific during spring and autumn, respectively. This study analyses the chemical composition and optical properties of PM

International audience

In this study, we assessed the feasibility of using ordinary face masks as a sampling means to collect airborne polycyclic aromatic hydrocarbons (PAHs). Nonwoven fabric masks can trap three-ring or larger PAHs at a high efficiency (>70%) and naphthalene at ∼17%. The sampling method is quantitative as confirmed by comparison with the standard method of the National Institute for Occupational Safety and Health. In conjunction with sensitive fluorescence detection, the method was applied to quantify nine airborne PAHs in a range of indoor and outdoor environments. Wearing the mask for 2 h allowed quantification of individual PAHs as low as 0.07 ng/m3. The demonstration shows applicability of the method in monitoring PAHs down to ∼30-80 ng/m3 in university office and laboratory settings and up to ∼900 ng/m3 in an incense-burning temple. Compared with traditional filter-/sorbent tube-based approaches, which require a sampling pump, our new method is simple, convenient, and inexpensive. More importantly, it closely tracks human exposure down to the individual level, thus having great potential to facilitate routine occupational exposure monitoring and large-scale surveillance of PAH concentrations in indoor and outdoor environments.

Traffic-related air pollutants (TRAPs) pose a serious health hazard for residents and commuters in urban areas. In this study, a real-time mobile monitoring system was deployed in Taipei, a typical East Asian city with an overlap of high population density, traffic, and special structures (e.g., viaducts), to capture the on-road TRAPs at different times of the day. In general, black carbon, ultrafine particles (UFPs), CO concentrations, and lung deposition surface area (LDSA) were positively correlated with traffic flow, and for PM2.5, a more independent fluctuating concentration was observed. During rush-hour periods, the mean concentrations of UFPs, PM2.5, and LDSA were 6.12 × 104 ± 3.83 × 104 cm−3, 23 ± 8 μg/m3, and 2.29 × 102 ± 1.20 × 102 μm2/cm3, respectively. Additionally, the UFP number concentration and LDSA were two times higher along the high-traffic commuting route than along the lower traffic route. Pollutants tended to accumulate at sites near viaducts and high buildings and were significantly influenced by vehicle composition. In this study, the ratio of LDSA to total particle surface area concentration was used as an indicator of the degree of particle irregularity, which was directly related to aging during transport.

International audience; Nitrous acid (HONO) is an important radical precursor that can impact secondary pollutant levels, especially in urban environments. Due to uncertainties in its heterogeneous formation mechanisms, models often under predict HONO concentrations. A number of heterogeneous sources at the ground have been proposed but there is no consensus about which play a significant role in the urban boundary layer. We present a new one-dimensional chemistry and transport model which performs surface chemistry based on molecular collisions and chemical conversion, allowing us to add detailed HONO formation chemistry at the ground. We conducted model runs for the 2010 CalNex campaign, finding good agreement with observations for key species such as O3, NOx, and HOx. With the ground sources implemented, the model captures the diurnal and vertical profile of the HONO observations. Primary HOx production from HONO photolysis is 2–3 times more important than O3 or HCHO photolysis at mid-day, below 10 m. The HONO concentration, and its contribution to HOx, decreases quickly with altitude. Heterogeneous chemistry at the ground provided a HONO source of 2.5 × 1011 molecules cm−2 s−1 during the day and 5 × 1010 molecules cm−2 s−1 at night. The night time source was dominated by NO2 hydrolysis. During the day, photolysis of surface HNO3/nitrate contributed 45%–60% and photo-enhanced conversion of NO2 contributed 20%–45%. Sensitivity studies addressing the uncertainties in both photolytic mechanisms show that, while the relative contribution of either source can vary, HNO3/nitrate is required to produce a surface HONO source that is strong enough to explain observations.

East Asian dust episodes have a multitude of impacts, including on human health, environment, and climate over near-source and receptor regions. However, the mechanistic understanding of the synoptic conditions of these outbreaks at different altitude layers, and their eventual environmental impacts are less studied. The present study analyzed the synoptic transport patterns of East Asian dust during multiple dust generation episodes that occurred over only a few days apart in northern China, and which eventually delivered high PM

Source-apportioned particle concentrations are necessary to properly evaluate the health impacts of air pollution. In this study, a measurement station was established at an urban roadside in northern Taiwan to the investigate lung deposited surface area (LDSA) concentration, a relevant metric for the adverse health effects of aerosol exposure, along with PM

Light-absorbing organic carbon (or brown carbon, BrC) has been recognized as a critical driver in regional-to-global climate change on account of its significant contribution to light absorption. BrC sources vary from primary combustion processes (burning of biomass, biofuel, and fossil fuel) to secondary formation in the atmosphere. This paper investigated the light-absorbing properties of BrC such as site-specific mass absorption cross-section (MACBrC), absorption Angstrom exponent (AAEBrC), and the absorbing component of the refractive index (kBrC) by using light absorption measurements from a 7-wavelength aethalometer over an urban environment of Chiang Mai, Thailand in northern peninsular Southeast Asia (PSEA), from March to April 2016. The contribution of BrC to total aerosol absorption (mean ± SD) was 46 ± 9%, 29 ± 7%, 24 ± 6%, 20 ± 4%, and 15 ± 3% at 370, 470, 520, 590, and 660 nm, respectively, highlighting the significant influence of BrC absorption on the radiative imbalance over northern PSEA. Strong and significant associations between BrC light absorption and biomass-burning (BB) organic tracers highlighted the influence of primary BB emissions. The median MACBrC and kBrC values at 370 nm were 2.4 m2 g−1 and 0.12, respectively. The fractional contribution of solar radiation absorbed by BrC relative to BC (mean ± SD) in the 370–950 nm range was estimated to be 34 ± 7%, which can significantly influence the regional radiation budget and consequently atmospheric photochemistry. This study provides valuable information to understand BrC absorption over northern PSEA and can be used in model simulations to reassess the regional climatic impact with greater accuracy.

Atmospheric humic-like substances (HULIS) are important components of biomass-burning (BB) emissions and highly associated with light-absorbing organic aerosols (often referred to as brown carbon). This study highlights the importance of BB-emitted HULIS aerosols in peninsular Southeast Asian outflow to the subtropical western North Pacific. We determined various key light-absorbing characteristics of HULIS i.e. mass absorption cross-section (MACHULIS), absorbing component of the refractive index (kHULIS), and absorption Angstrom exponent (AAEHULIS) based on ground-based aerosol light absorption measurements along with HULIS concentrations in springtime aerosols at Lulin Atmospheric Background Station (LABS; 2862 m above mean sea level), which is a representative high-altitude remote site in the western North Pacific. Daily variations of HULIS (0.58–12.92 μg m−3) at LABS were mostly linked with the influence from incoming air-masses, while correlations with BB tracers and secondary aerosols indicated the attribution of primary and secondary sources. Stronger light absorption capability of HULIS was clearly evident from MACHULIS and kHULIS values at 370 nm, which were about ~1.5 times higher during BB-dominated days (1.16 ± 0.75 m2 g−1 and 0.05 ± 0.03, respectively) than that during non-BB days (0.77 ± 0.89 m2 g−1 and 0.03 ± 0.04, respectively). Estimates from a simple radiative transfer model showed that HULIS absorption can add as much as 15.13 W g−1 to atmospheric warming, and ~46% more during BB-dominated than non-BB period, highlighting that HULIS light absorption may significantly affect the Earth–atmosphere system and tropospheric photochemistry over the western North Pacific.

Volcanic eruptions are important natural sources of gases and aerosols to the environment. However, their impact on the global cycle of trace elements, including mercury (Hg), remains poorly understood. On 9 April 2021, La Soufriere volcano (13.33°N, 61.18°W) erupted in the Caribbean Sea. Ozone Monitoring Instrument (OMI) measurements of sulfur dioxide (SO2) tracked the transport of volcanic SO2 in the troposphere over long distances from the source, including to the western North Pacific ∼10 day after eruption. A spike in gaseous and particle-bound mercury concentrations along with a peak in aerosol back-scattering coefficient at Lulin Atmospheric Background Station (LABS, 23.47°N, 120.87°E; 2862 m AMSL) coincided with the volcanic plume transport on 19 April. The slope of gaseous elemental mercury vs. carbon monoxide concentrations during the event was 0.027, which is distinctly higher than for Southeast Asia biomass burning (slope = 0.005) and East Asia outflow (0.011) pollution sources. Arrival of the plume high above Taiwan was confirmed by significant changes in signature aerosol properties. Thus, with critical observational evidence, our study reported for the first time enhanced mercury levels ∼18000 km downwind from a volcano source, providing an important check on volcanic Hg emission strength.

In this study, we investigated the influences of stratospheric intrusion (SI) on the tropospheric ozone (O3) at Lulin Atmospheric Background Station (LABS, 2862 m MSL), a representative high-altitude site in East Asia. Thresholds for surface O3, carbon monoxide (CO), and relative humidity (RH) were set to identify SI events at LABS. Accordingly, 3.0% of the observation period was impacted by SI leading to a net O3 enhancement of 14.6 ± 9.6 ppb at LABS. Factors influencing the two most common SI event types affecting LABS, i.e. tropopause folds (major) and tropical cyclones (minor), were discussed. We utilized ERA5 reanalysis products (meteorology and O3) to trace and analyze the pathway and mechanism of these SI types over sub-tropical East Asia. With a conceptual model, we illustrate two driving circulations for SI air at ∼200 hPa that affect subtropical East Asia. SI air generated due to Rossby wave breaks are transported equatorward and downward into the troposphere. The southern westerlies passing south of the Tibetan Plateau can further push the SI air eastward. A SI event in 2007 with a significant O3 enhancement of 43.4 ppb caused by typhoon Nari was detected and discussed to depict the second SI type.

Many aromatic compounds (e.g., polycyclic aromatic hydrocarbons (PAHs)) found in atmospheric aerosols are toxic and exist in both unsubstituted and substituted forms. Previous studies have mainly concentrated on investigating unsubstituted PAHs, leaving the substituted compounds largely uncharacterized. This study focuses on detection of both unsubstituted and substituted aromatics in ambient aerosol samples using ultrahigh-resolution mass spectrometry. Aerosol samples collected from roadside, urban, and suburban sites in Hong Kong were characterized by Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) coupled with atmospheric pressure photoionization (APPI) or electrospray ionization (ESI). In the APPI+ mode, 166 aromatic CH formulas (i.e., formulas containing C and H only and with a double bond equivalent (DBE) of 4 or higher) were determined through molecular formula calculations based on an accurate m/z determination. Among the determined aromatic CH formulas, 141 are possible alkylated monocyclic aromatic hydrocarbon (MAH) or PAH formulas, and account for ≥ 45% of the total intensity by aromatic CH+ formulas. Both APPI+ and ESI+ are effective in detecting nitroaromatics (i.e., CHO2N1 formulas and DBE ≥ 5). The two ionization modes provide complementary formula coverage, with formulas determined by APPI+ extending to higher DBE and those by ESI+ covering higher carbon numbers. Alkylated nitrobenzene compounds are the most abundant among nitroaromatics, and they, together with alkylated nitro-PAHs, account for > 80% of the total intensity of aromatic CHO2N+ formulas, indicating the importance of these compounds in real aerosol samples. Aromatic CHN+ and CHO+ formulas are also determined, confirming the atmospheric presence of some previously reported O- and N-containing aromatic compounds and revealing new possible formulas. The determination of aromatic organic formulas in this study provides useful guidance for future quantitative analysis of hazardous aromatic compounds. Future work is needed to determine the abundance and to study the toxicity of alkylated MAHs and PAHs outside the 16 US EPA priority PAH compounds.

Despite many demonstrated benefits that biochars can have on agricultural soils, there are few examples of profitable biochar utilization on commercial farms. Barriers to profitability include successfully pairing waste streams, production facilities, and farms where biochar is utilized. However, farm-scale biochar systems, which utilize agricultural wastes as feedstocks and produce energy and biochar for on-farm use, may have efficiency advantages over regional, industrial biochar production. Two critical uncertainties for the feasibility of on-farm production are 1) whether a biochar can be produced from on-farm feedstocks with appropriate qualities for soil amendment, and 2) whether on-farm feedstocks are sufficiently abundant to meet on-farm demand. Here we evaluate these issues for a farm-scale gasification system in NE Washington State that produces biochar from grass seed screenings and straw. Field trials to evaluate the biochar as a liming alternative found it was highly effective when broadcast at a rate of at least 18 Mg ha−1. Biochar outperformed hydrated lime in the first year of the study and improved yields by a factor of 2.88 across both years. Biochar produced from on-farm feedstocks were sufficient to amend 6.3–11.8% of the production area annually, translating to a return interval of 9–16 years. Potential co-production of electrical power far exceeded on-farm demand for operating a seed cleaning mill. We conclude that an on-farm biochar production system is physically feasible for meeting demands for both power and liming amendments.

In this study, the trends and factors influencing wintertime precipitation chemistry at a remote site downwind of continental East Asia were investigated. A total of 336 precipitation samples were collected from 2005 to 2019 at Pengjia Islet, a site ~56 km north of the main island of Taiwan. Overall, the samples had a volume-weighted mean pH of 4.81 (ranging from 3.03 to 7.00), with 74% of samples considered as acid rain (pH

East Asian Dust (EAD) has had a measurable impact on global climate and air quality, including visibility and human health, in numerous locations around the globe over the past decade. The accuracy of an air quality modeling system to simulate dust events is vital for early warning systems. The most significant dust event observed in 6 years for northern Taiwan occurred during 4th–9th April 2018, and was characterized by high wind speeds (9–13 m s−1) upon arrival to the region. We assessed the windblown dust emission treatment across various modifications and found better model performance by decreasing the soil moisture factor and updating the aerosol speciation profile over East Asia. In the optimized CMAQ simulation, uplifted dust particles reached a maximum height of 500–700 hPa, which is crucial for effective transport of the dust plume to the downwind Taiwan region. However, by tracking the vertical distribution profile, we found the model was insufficient to estimate dust aerosol after exiting from over the continent and entering the marine boundary layer. Our simulation indicated the dust event consisted of two plumes, where the first one was significantly impacted by wet deposition (−70.65%) from a rainfall belt stretching across Japan, Korea and the East China Sea. Then, low wind speed during a period of no precipitation over the marine area led to even greater dust deposition (−89.11%) from the second plume, resulting in a consistent negative bias for the simulation. This modeling study highlights the importance of improving the dust emission treatment for a better simulation of dust aerosol transport over the marine boundary layer. To reduce the uncertainty in the dust outflow region, the deposition mechanisms for the CMAQ dust treatment should be revised.

Knowledge of the relative abundance of primary organic aerosol (POA) and secondary organic aerosol (SOA) forms an important scientific basis for formulating particulate matter (PM) control policies. Taking advantage of a comprehensive chemical composition data set of PM2.5 including both POA and SOA tracers (most notably, SOA tracers of a few biogenic voltaic organic compound precursors), we investigate the impact of inclusion of SOA tracers on the source apportionment of organic carbon (OC) and PM2.5 in the Pearl River Delta region of China using positive matrix factorization (PMF). In PMF runs incorporating SOA tracers (PMFw), ten PMF factors were resolved including four secondary factors: (1) SOA I (α-pinene, β-caryophyllene, and naphthalene-derived SOA), (2) SOA II (isoprene-derived SOA), (3) a secondary sulfate factor, and (4) a secondary nitrate factor. In PMF tests without SOA tracers (PMFwo), the SOA I and SOA II factors could not be extracted, but the remaining eight source factors were resolved....

Gas-phase biogenic volatile organic compounds (BVOCs) are oxidized in the troposphere to produce secondary pollutants such as ozone (O3), organic nitrates (RONO2), and secondary organic aerosol (SOA). Two coupled zero-dimensional models have been used to investigate differences in oxidation and SOA production from isoprene and α-pinene, especially with respect to the nitrate radical (NO3), above and below a forest canopy in rural Michigan. In both modeled environments (above and below the canopy), NO3 mixing ratios are relatively small (3 contributes 12 % of total daytime α-pinene oxidation below the canopy while only contributing 4 % above. Increasing background pollutant levels to simulate a more polluted suburban or peri-urban forest environment increases the average contribution of NO3 to daytime below-canopy α-pinene oxidation to 32 %. Gas-phase RONO2 produced through NO3 oxidation undergoes net transport upward from the below-canopy environment during the day, and this transport contributes up to 30 % of total NO3-derived RONO2 production above the canopy in the morning (∼ 07:00). Modeled SOA mass loadings above and below the canopy ultimately differ by less than 0.5 µg m−3, and extremely low-volatility organic compounds dominate SOA composition. Lower temperatures below the canopy cause increased partitioning of semi-volatile gas-phase products to the particle phase and up to 35 % larger SOA mass loadings of these products relative to above the canopy in the model. Including transport between above- and below-canopy environments increases above-canopy NO3-derived α-pinene RONO2 SOA mass by as much as 45 %, suggesting that below-canopy chemical processes substantially influence above-canopy SOA mass loadings, especially with regard to monoterpene-derived RONO2.

Fine particulate matter (PM) is capable of scattering and absorbing light and is the main culprit of visibility degradation. Major PM chemical components have been characterized for their light absorption and scattering efficiency, but separating the organic components has yet to be fully parameterized with light extinction coefficients. In this study, light extinction data and PM2.5 chemical composition data were monitored at a suburban site in Hong Kong over a two-year period (2013-2014). Using the IMPROVE formula to reconstruct the light scattering coefficient under-estimates the measured scattering coefficient (slope=0.85), but explains the data variability well (R2: 0.92). A multilinear regression analysis using the 'local' PM2.5 composition data and measured extinction coefficients was performed to empirically establish mass scattering and absorption efficiencies (i.e., MSE and MAE) for the different PM2.5 components. During this process, the stepwise separation of organic matter (OM) was performed according to water solubility: water soluble organic carbon (WSOC) and water insoluble organic carbon (WISOC); then according to water affinity: hydrophilic carbon (HPI) and hydrophobic carbon (HPO), the latter being the sum of humic-like substance carbon (HULISc) and WISOC. The localized formulas predict the measured extinction coefficients (i.e., σsp and σap) very well (slope=0.99 for both). The results showed that the dry MSE of ammonium sulfate and ammonium nitrate were comparable with those used in the IMPROVE equation while MSE for OC is noticeably larger in the localized formula (13.1 vs. 7.2m2g-1). Splitting the OM into different fractions revealed the MSE for hydrophilic carbon (16.1m2g-1) was distinctly higher than for hydrophobic carbon, including HULIS (11.0m2g-1) and WISOC (12.8m2g-1). Regression analysis of light absorption against EC and OC indicates that absorption is not fully accounted for considering only EC. OC also contributes to light absorption.

The formation of sulfate (SO42−) in the atmosphere is linked chemically to its direct precursor, sulfur dioxide (SO2), through several key oxidation paths for which nitrogen oxides or NOx (NO and NO2) play essential roles. Here we present a coherent description of the dependence of SO42– formation on SO2 and NOx under haze-fog conditions, in which fog events are accompanied by high aerosol loadings and fog-water pH in the range of 4.7–6.9. Three SO42– formation regimes emerge as defined by the role played by NOx. In the low-NOx regime, NOx act as catalyst for HOx, which is a major oxidant for SO2, whereas in the high-NOx regime, NO2 is a sink for HOx. Moreover, at highly elevated NOx levels, a so-called NO2-oxidant regime exists in which aqueous NO2 serves as the dominant oxidant of SO2. This regime also exists under clean fog conditions but is less prominent. Sensitivity calculations using an emission-driven box model show that the reduction of SO42– is comparably sensitive to the reduction of SO2 and NOx emissions in the NO2-oxidant regime, suggesting a co-reduction strategy. Formation of SO42− is relatively insensitive to NOx reduction in the low-NOx regime, whereas reduction of NOx actually leads to increased SO42– production in the intermediate high-NOx regime. Distinct dependence of atmospheric SO42– formation on NOx levels in haze-fog events is revealed by SO42– production isopleths that are obtained through simulations of atmospheric chemistry with a box model.

Long-range pollution transport (LRT) events have a wide impact across East Asia, but are often difficult to track due to imprecise emission inventories and changing domain scales as the plume moves from source to receptor locations. This study adjusts a bottom-up emission inventory based on changes in remotely sensed NO2 column densities for a source region of East Asia, then with CMAQv5.2.1 simulates transport of LRT plumes to Taiwan. Adjustment of an emissions inventory based on satellite measurements during the COVID-19 lockdown in China led to a ~59% reduction in emissions over the relevant source area in China compared to base emissions. As a result, PM2.5 mass concentrations were reproduced to match observations (mean fractional bias, MFB of –13.9% and 18.5% at a remote and urban station) as the plume passed through northern Taiwan. Furthermore, the OMI-adjusted emissions simulation brought all of the major PM2.5 components to within ~50% of the measured values. Another LRT event from 2018 with more subtle OMI-adjustments to the emissions was also simulated and with improved overall PM2.5 mass concentration at the northern tip of Taiwan (MFB: –91.5%) compared to the base model (MFB: –102.1%), and an acceptable index of agreement (0.78). For the 2018 event, non sea-salt sulfate concentrations were consistently underpredicted (0.2–0.4), while nitrate concentrations were overpredicted by up to factor of 11. Copernicus Atmosphere Monitoring Service (CAMS) reanalysis of the PM2.5 concentrations shows high sulfate concentrations in eastern China in the areas associated with 72-h back-trajectories from northern Taiwan during both events, lending support for future model investigations of sulfate source area production and transport to Taiwan. In order to better track these LRT events out of East Asia and optimize OMI-adjustment methodology, it is recommended to explore other satellite-based products to map unaccounted for SO2 sources upstream of Taiwan.

Planetary boundary layer height (PBLH) is often used to characterize the structure of the lower atmosphere. Aerosol lidar, a ground-based remote sensing method, provides the vertical distribution of aerosol at a high temporal resolution observation data, from which, the PBL structure and the position of the PBL top can be comprehensively studied. PBLH determination with lidar data depends primarily on the characteristic turbulent motions in the atmosphere and the geophysical location. However, lidar determination of PBLH over densely populated subtropical locations has rarely been discussed; thus, developing retrieval techniques suitable to these areas is necessary. In this study, four PBLH determination methods (Gradient, δ–threshold, Haar wavelet transform, and hybrid image processing) are applied to estimate the PBLH from lidar observations over an urban area in East Asia, and one—the Gradient method—relied on potential temperature measurements from an unmanned aerial vehicle (UAV) flights to validate our results. Our results indicate that a combination of the gradient method and δ-threshold method can provide better results, in terms of diurnal pattern, than using either method individually. Furthermore, the Haar wavelet and the Hybrid image processing can detect the PBL development comparably well, but both methods are dependent on their initial conditions and optimized algorithm settings. In addition, the accompanying UAV observations are conclusively shown to have a high degree of efficacy for validating the lidar data. This research highlights that a combination of PBLH determination methods can better describe the PBLH evolution throughout a day in some cases, while in others less common determination methods are proving useful, and a suite of retrieval methods should still be explored for precisely mapping the PBL in densely populated subtropical areas.

Single Particle Aerosol Mass Spectrometers (SPAMS) have been increasingly deployed for aerosol studies in Asia. To date, SPAMS is most often used to provide unscaled information for both the size and chemical composition of individual particles. The instrument's lack of accuracy is primarily due to only a fraction of particles being detected after collection, and the instrumental sensitivity is un-calibrated for various chemical species in mixed ambient aerosols. During a campaign from January to April 2013 at a coastal site in Hong Kong, the particle number information and ion intensity of major PM 2.5 components collected by SPAMS were scaled by comparing with collocated bulk PM 2.5 measurements of hourly or higher resolution. The bulk measurements include PM 2.5 mass by a SHARP 5030 Monitor, major ions by a Monitor for Aerosols & Gases in ambient Air (MARGA), and organic carbon (OC) and elemental carbon (EC) by a Sunset OCEC analyzer. During the data processing, both transmission efficiency (scaled with the Scanning Mobility Particle Sizer) and hit efficiency conversion were considered, and component ion intensities quantified as peak area (PA) and relative peak area (RPA) were analyzed to track the performance. The comparison between the scaled particle mass assuming a particle density of 1.9 g cm −3 from SPAMS and PM 2.5 concentration showed good correlation (R 2 = 0.81) with a slope of 0.814 ± 0.004. Regression analysis results suggest an improved scaling performance using RPA compared with PA for most of the major PM 2.5 components, including sulfate, nitrate, potassium, ammonium, OC and EC. Thus, we recommend preferentially scaling these species using the RPA. For periods of high K + concentrations (>1.5 μg m −3 ), under-estimation of K + by SPAMS was observed due to exceeding the dynamic range of the acquisition board. When only applying the hit efficiency correction, data for sulfate, nitrate, ammonium, potassium and OC were in reasonably good correlation (R 2 = 0.56–0.79) with the bulk measurements, suggesting semi-quantified data by the hit efficiency correction can be utilized when transmission efficiency correction is not available. More inter-comparisons of this type are needed to assess the inter-instrument variability among different SPAMS instruments.

International audience; Measurements of hydroxyl (OH) and hydroperoxy (HO2*) radical concentrations were made at the Pasadena ground site during the CalNex-LA 2010 campaign using the laser-induced fluorescence-fluorescence assay by gas expansion technique. The measured concentrations of OH and HO2* exhibited a distinct weekend effect, with higher radical concentrations observed on the weekends corresponding to lower levels of nitrogen oxides (NOx). The radical measurements were compared to results from a zero-dimensional model using the Regional Atmospheric Chemical Mechanism-2 constrained by NOx and other measured trace gases. The chemical model overpredicted measured OH concentrations during the weekends by a factor of approximately 1.4 ± 0.3 (1σ), but the agreement was better during the weekdays (ratio of 1.0 ± 0.2). Model predicted HO2* concentrations underpredicted by a factor of 1.3 ± 0.2 on the weekends, while measured weekday concentrations were underpredicted by a factor of 3.0 ± 0.5. However, increasing the modeled OH reactivity to match the measured total OH reactivity improved the overall agreement for both OH and HO2* on all days. A radical budget analysis suggests that photolysis of carbonyls and formaldehyde together accounted for approximately 40% of radical initiation with photolysis of nitrous acid accounting for 30% at the measurement height and ozone photolysis contributing less than 20%. An analysis of the ozone production sensitivity reveals that during the week, ozone production was limited by volatile organic compounds throughout the day during the campaign but NOx limited during the afternoon on the weekends.

Long-range transport (LRT) of air pollutants from East Asia during the northeast monsoon season impacts several downwind locations. In 2020, the initial COVID-19 lockdowns in China overlapped with Week 3 of the Chinese New Year (CNY) holiday, and an Asian outflow event. Thus, movement of the Chinese populace from city to city was already greatly reduced by the time of the LRT episode, although the reductions in industrial output are less clear. We found NO2 column concentrations were reduced by 24% during the CNY Week 3 this year compared to previous years. The attenuated transport event arrived to northern Taiwan with a PM2.5 concentration, Graphical abstract Unlabelled Image, Highlights • COVID-19 lockdown in China reduced long-range transport of air pollution to Taiwan. • OMI NO2 over central-north China reduced by 24% compared to previous years. • PM2.5 concentration in northern Taiwan 2 times lower compared to similar episode • CMAQ simulation with 50% reduced emission in China matches measured PM2.5 in Taiwan. • Avoided PM2.5 pollution equivalent to 0.5 μg m−3 reduction for entire winter season