Elemental Characterization of Ambient Particulate Matter for a Globally Distributed Monitoring Network: Methodology and Implications.

Global ground-level measurements of elements in ambient particulate matter (PM) can provide valuable information to understand the distribution of dust and trace elements, assess health impacts, and investigate emission sources. We use X-ray fluorescence spectroscopy to characterize the elemental composition of PM samples collected from 27 globally distributed sites in the Surface PARTiculate mAtter Network (SPARTAN) over 2019-2023. Consistent protocols are applied to collect all samples and analyze them at one central laboratory, which facilitates comparison across different sites. Multiple quality assurance measures are performed, including applying reference materials that resemble typical PM samples, acceptance testing, and routine quality control. Method detection limits and uncertainties are estimated. Concentrations of dust and trace element oxides (TEO) are determined from the elemental dataset. In addition to sites in arid regions, a moderately high mean dust concentration (6 µg/m3) in PM2.5 is also found in Dhaka (Bangladesh) along with a high average TEO level (6 µg/m3). High carcinogenic risk (>1 cancer case per 100000 adults) from airborne arsenic is observed in Dhaka (Bangladesh), Kanpur (India), and Hanoi (Vietnam). Industries of informal lead-acid battery and e-waste recycling as well as coal-fired brick kilns likely contribute to the elevated trace element concentrations found in Dhaka.

Use of portable air cleaners to reduce aerosol transmission on a hospital coronavirus disease 2019 (COVID-19) ward.

OBJECTIVE: To study the airflow, transmission, and clearance of aerosols in the clinical spaces of a hospital ward that had been used to care for patients with coronavirus disease 2019 (COVID-19) and to examine the impact of portable air cleaners on aerosol clearance. DESIGN: Observational study. SETTING: A single ward of a tertiary-care public hospital in Melbourne, Australia. INTERVENTION: Glycerin-based aerosol was used as a surrogate for respiratory aerosols. The transmission of aerosols from a single patient room into corridors and a nurses' station in the ward was measured. The rate of clearance of aerosols was measured over time from the patient room, nurses' station and ward corridors with and without air cleaners [ie, portable high-efficiency particulate air (HEPA) filters]. RESULTS: Aerosols rapidly travelled from the patient room into other parts of the ward. Air cleaners were effective in increasing the clearance of aerosols from the air in clinical spaces and reducing their spread to other areas. With 2 small domestic air cleaners in a single patient room of a hospital ward, 99% of aerosols could be cleared within 5.5 minutes. CONCLUSIONS: Air cleaners may be useful in clinical spaces to help reduce the risk of acquisition of respiratory viruses that are transmitted via aerosols. They are easy to deploy and are likely to be cost-effective in a variety of healthcare settings.

Air quality and health impact of 2019-20 Black Summer megafires and COVID-19 lockdown in Melbourne and Sydney, Australia.

Poor air quality is an emerging problem in Australia primarily due to ozone pollution events and lengthening and more severe wildfire seasons. A significant deterioration in air quality was experienced in Australia's most populous cities, Melbourne and Sydney, as a result of fires during the so-called Black Summer which ran from November 2019 through to February 2020. Following this period, social, mobility and economic restrictions to curb the spread of the COVID-19 pandemic were implemented in Australia. We quantify the air quality impact of these contrasting periods in the south-eastern states of Victoria and New South Wales (NSW) using a meteorological normalisation approach. A Random Forest (RF) machine learning algorithm was used to compute baseline time series' of nitrogen dioxide (NO2), ozone (O3), carbon monoxide CO and particulate matter with diameter < 2.5 µm (PM2.5), based on a 19 year, detrended training dataset. Across Victorian sites, large increases in CO (188%), PM2.5 (322%) and ozone (22%) were observed over the RF prediction in January 2020. In NSW, smaller pollutant increases above the RF prediction were seen (CO 58%, PM2.5 80%, ozone 19%). This can be partly explained by the RF predictions being high compared to the mean of previous months, due to high temperatures and strong wind speeds, highlighting the importance of meteorological normalisation in attributing pollution changes to specific events. From the daily observation-RF prediction differences we estimated 249.8 (95% CI: 156.6-343.) excess deaths and 3490.0 (95% CI 1325.9-5653.5) additional hospitalisations were likely as a result of PM2.5 and O3 exposure in Victoria and NSW. During April 2019, when COVID-19 restrictions were in place, on average NO2 decreased by 21.5 and 8% in Victoria and NSW respectively. O3 and PM2.5 remained effectively unchanged in Victoria on average but increased by 20 and 24% in NSW respectively, supporting the suggestion that community mobility reduced more in Victoria than NSW. Overall the air quality change during the COVID-19 lockdown had a negligible impact on the calculated health outcomes.

Aerosol generation related to respiratory interventions and the effectiveness of a personal ventilation hood.

OBJECTIVE: To quantify aerosol generation from respiratory interventions and the effectiveness of their removal by a personal ventilation hood. DESIGN AND SETTING: Determination of the aerosol particle generation (in a single, healthy volunteer in a clean room) associated with breathing, speaking, wet coughing, oxygen (O2) 15 L/min via face mask, O2 60 L/min via nasal prongs, bilevel non-invasive positive-pressure ventilation (BiPAP) and nebulisation with O2 10 L/min. INTERVENTIONS: Aerosol generation was measured with two particle sizer and counter devices, focusing on aerosols 0.5-5 µm (human-generated aerosols), with and without the hood. An increase from baseline of less than 0.3 particles per mL was considered a low level of generation. MAIN OUTCOME MEASURES: Comparisons of aerosol generation between different respiratory interventions. Effectiveness of aerosol reduction by a personal ventilation hood. RESULTS: Results for the 0.5-5 µm aerosol range. Quiet breathing and talking demonstrated very low increase in aerosols (< 0.1 particles/mL). Aerosol generation was low for wet coughing (0.1 particles/mL), O2 15 L/min via face mask (0.18 particles/mL), and high flow nasal O2 60 L/min (0.24 particles/mL). Non-invasive ventilation generated moderate aerosols (29.7 particles/mL) and nebulisation very high aerosols (1086 particles/mL); the personal ventilation hood reduced the aerosol counts by 98% to 0.5 particles/mL and 8.9 particles/mL respectively. CONCLUSIONS: In this human volunteer study, the administration of O2 15 L/min by face mask and 60 L/min nasal therapy did not increase aerosol generation beyond low levels. Non-invasive ventilation caused moderate aerosol generation and nebulisation therapy very high aerosol generation. The personal ventilation hood reduced the aerosol counts by at least 98%.

Surface ozone exceedances in Melbourne, Australia are shown to be under NOx control, as demonstrated using formaldehyde:NO2 and glyoxal:formaldehyde ratios.

Two and a half years of multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of nitrogen dioxide (NO2), formaldehyde (HCHO) and glyoxal (CHOCHO) are presented alongside in-situ ozone (O3) measurements in Melbourne, Australia. Seasonal and diurnal cycles, vertical profiles and relationships with key meteorological variables are provided. NO2 and CHOCHO were found at highest concentration for low wind speeds implying that their sources were predominantly localised and anthropogenic. HCHO showed an exponential relationship with temperature and a strong wind direction dependence from the northern and eastern sectors, and therefore most likely originated from oxidation of biogenic volatile organic compounds (VOCs) from surrounding forested and rural areas. The glyoxal:formaldehyde ratio (Rgf), reported for the first time in Australia, was consistently high compared to values elsewhere in the world with a mean of 0.105 ± 0.0503 and tended to increase with increasing anthropogenic influence. The HCHO:NO2 ratio (Rfn) was used to characterise tropospheric ozone formation conditions. A strong relationship was found between high temperature, low Rgf, high Rfn and high ozone surface concentrations. Therefore, we propose that both Rgf and Rfn may be useful indicators of tropospheric ozone production regimes and concentrations. The Rfn showed that the vast majority of high ozone production episodes occurred under NOx-limited conditions, suggesting that surface ozone pollution events in Melbourne could be curtailed using NOx emission controls.

A global analysis of urban design types and road transport injury: an image processing study.

BACKGROUND: Death and injury due to motor vehicle crashes is the world's fifth leading cause of mortality and morbidity. City and urban designs might play a role in mitigating the global burden of road transport injury to an extent that has not been captured by traditional safe system approaches. We aimed to determine the relationship between urban design and road trauma across the globe. METHODS: Applying a combined convolutional neural network and graph-based approach, 1692 cities capturing one third of the world's population were classified into types based on urban design characteristics represented in sample maps. Associations between identified city types, characteristics contained within sample maps, and the burden of road transport injury as measured by disability adjusted life-years were estimated through univariate and multivariate analyses, controlling for the influence of economic activity. FINDINGS: Between Mar 1, 2017, and Dec 24, 2018, nine global city types based on a final sample of 1632 cities were identified. Burden of road transport injury was an estimated two-times higher (risk ratio 2·05, 95% CI 1·84-2·27) for the poorest performing city type compared with the best performing city type, culminating in an estimated loss of 8·71 (8·08-9·25) million disability-adjusted life-years per year attributable to suboptimal urban design. City types that featured a greater proportion of railed public transport networks combined with dense road networks characterised by smaller blocks showed the lowest rates of road traffic injury. INTERPRETATION: This study highlights the important role that city and urban design plays in mitigating road transport injury burden at a global scale. It is recommended that road and transport safety efforts promote urban design that features characteristics inherent in identified high-performance city types including higher density road infrastructure and high rates of public transit. FUNDING: See acknowledgments.

Characterization of aerosols over the Great Barrier Reef: The influence of transported continental sources.

The rapid environmental changes in Australia prompt a more thorough investigation of the influence of transportation, local emissions, and optical-chemical properties on aerosol production across the region. A month-long intensive measurement campaign was conducted during spring 2016 at Mission Beach, a remote coastal site west of the Great Barrier Reef (GBR) on the north-east coast of Australia. One aerosol pollution episode was investigated in early October. This event was governed by meteorological conditions and characterized by the increase in black carbon (BC) mass concentration (averaged value of 0.35 ±â€¯0.20 µg m-3). Under the influence of the continental transportation, a new layer of nucleation-mode aerosols with an initial size diameter of 20 nm was observed and aerosol number concentrations reached the peak of 6733 cm-3 at a diameter of 29 nm. The averaged aerosol extinction coefficient at the height of 2 km was 150 Mm-1, with a small depolarized ratio (3.5-5%). Simultaneously, the boundary layer height presented a fall-rise trend in the presence of these enhanced aerosol concentrations and became stable in a later stage of the episode. We did not observe clear boundary layer height diurnal variations from the LiDAR observations or from the Weather Research and Forecasting (WRF) model outputs, except in an earlier stage of the aerosol episode for the former. Although the sea breeze may have been responsible for these particles, on the balance of available data, we suggest that the aerosol properties at the GBR surface during this period are more likely influenced by regional transportation of continental sources, including biomass-burning aerosols.

The influence of mixing on stratospheric age of air changes in the 21st century.

Climate models consistently predict an acceleration of the Brewer-Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among individual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyze the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyze the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesized to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10% to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.

Tropospheric ozone in CCMI models and Gaussian process emulation to understand biases in the SOCOLv3 chemistry-climate model.

Previous multi-model intercomparisons have shown that chemistry-climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC/IGAC (Stratosphere-troposphere Processes and their Role in Climate/International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40-50% in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ~30% in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU - approximately 33% larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, "SOCOLv3.1", which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds) are responsible for more than 90% of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20% more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry-climate models.

Microbial mercury methylation in Antarctic sea ice.

Atmospheric deposition of mercury onto sea ice and circumpolar sea water provides mercury for microbial methylation, and contributes to the bioaccumulation of the potent neurotoxin methylmercury in the marine food web. Little is known about the abiotic and biotic controls on microbial mercury methylation in polar marine systems. However, mercury methylation is known to occur alongside photochemical and microbial mercury reduction and subsequent volatilization. Here, we combine mercury speciation measurements of total and methylated mercury with metagenomic analysis of whole-community microbial DNA from Antarctic snow, brine, sea ice and sea water to elucidate potential microbially mediated mercury methylation and volatilization pathways in polar marine environments. Our results identify the marine microaerophilic bacterium Nitrospina as a potential mercury methylator within sea ice. Anaerobic bacteria known to methylate mercury were notably absent from sea-ice metagenomes. We propose that Antarctic sea ice can harbour a microbial source of methylmercury in the Southern Ocean.