On Nucleation Pathways and Particle Size Distribution Evolutions in Stratospheric Aircraft Exhaust Plumes with H2SO4 Enhancement.

Stratospheric aerosol injection (SAI) is proposed as a means of reducing global warming and climate change impacts. Similar to aerosol enhancements produced by volcanic eruptions, introducing particles into the stratosphere would reflect sunlight and reduce the level of warming. However, uncertainties remain about the roles of nucleation mechanisms, ionized molecules, impurities (unevaporated residuals of injected precursors), and ambient conditions in the generation of SAI particles optimally sized to reflect sunlight. Here, we use a kinetic ion-mediated and homogeneous nucleation model to study the formation of H2SO4 particles in aircraft exhaust plumes with direct injection of H2SO4 vapor. We find that under the conditions that produce particles of desired sizes (diameter ∼200-300 nm), nucleation occurs in the nascent (t < 0.01 s), hot (T = 360-445 K), and dry (RH = 0.01-0.1%) plume and is predominantly unary. Nucleation on chemiions occurs first, followed by neutral new particle formation, which converts most of the injected H2SO4 vapor to particles. Coagulation in the aging and diluting plumes governs the subsequent evolution to a narrow (σg = 1.3) particle size distribution. Scavenging by exhaust soot is negligible, but scavenging by acid impurities or incomplete H2SO4 evaporation in the hot exhaust plume and enhanced background aerosols can matter. This research highlights the need to obtain laboratory and/or real-world experiment data to verify the model prediction.

Environmental exposure disparities in ultrafine particles and PM2.5 by urbanicity and socio-demographics in New York state, 2013-2020.

BACKGROUND: The spatiotemporal and demographic disparities in exposure to ultrafine particles (UFP; number concentrations of particulate matter (PM) with diameter ≤0.1 µm), a key subcomponent of fine aerosols (PM2.5; mass concentrations of PM ≤ 2.5 µm), have not been well studied. OBJECTIVE: To quantify and compare the aerosol pollutant exposure disparities for UFP and PM2.5 by socio-demographic factors in New York State (NYS). METHODS: Ambient atmospheric UFP and PM2.5 were quantified using a global three-dimensional model of chemical transport with state-of-the-science aerosol microphysical processes validated extensively with observations. We matched these to U.S. census demographic data for varied spatial scales (state, county, county subdivision) and derived population-weighted aerosol exposure estimates. Aerosol exposure disparities for each demographic and socioeconomic (SES) indicator, with a focus on race-ethnicity and income, were quantified for the period 2013-2020. RESULTS: The average NYS resident was exposed to 4451 #·cm-3 UFP and 7.87 µg·m-3 PM2.5 in 2013-2020, but minority race-ethnicity groups were invariably exposed to greater daily aerosol pollution (UFP: +75.0% & PM2.5: +16.2%). UFP has increased since 2017 and is temporally and seasonally out-of-phase with PM2.5. Race-ethnicity exposure disparities for PM2.5 have declined over time; by -6% from 2013 to 2017 and plateaued thereafter despite its decreasing concentrations. In contrast, these disparities have increased (+12.5-13.5%) for UFP. The aerosol pollution exposure disparities were the highest for low-income minorities and were more amplified for UFP than PM2.5. DISCUSSION: We identified large disparities in aerosol pollution exposure by urbanization level and socio-demographics in NYS residents. Jurisdictions with higher proportions of race-ethnicity minorities, low-income residents, and greater urbanization were disproportionately exposed to higher concentrations of UFP and PM2.5 than other NYS residents. These race-ethnicity exposure disparities were much larger, more disproportionate, and unabating over time for UFP compared to PM2.5 across various income strata and levels of urbanicity.

Hidden danger: The long-term effect of ultrafine particles on mortality and its sociodemographic disparities in New York State.

Although previous studies have shown increased health risks of particulate matters, few have evaluated the long-term health impacts of ultrafine particles (UFPs or PM0.1, ≤ 0.1 µm in diameter). This study assessed the association between long-term exposure to UFPs and mortality in New York State (NYS), including total non-accidental and cause-specific mortalities, sociodemographic disparities and seasonal trends. Collecting data from a comprehensive chemical transport model and NYS Vital Records, we used the interquartile range (IQR) and high-level UFPs (≥75 % percentile) as indicators to link with mortalities. Our modified difference-in-difference model controlled for other pollutants, meteorological factors, spatial and temporal confounders. The findings indicate that long-term UFPs exposure significantly increases the risk of non-accidental mortality (RR=1.10, 95 % CI: 1.05, 1.17), cardiovascular mortality (RR=1.11, 95 % CI: 1.05, 1.18) particularly for cerebrovascular (RR=1.21, 95 % CI: 1.10, 1.35) and pulmonary heart diseases (RR=1.33, 95 % CI: 1.13, 1.57), and respiratory mortality (borderline significance, RR=1.09, 95 % CI: 1.00, 1.18). Hispanics (RR=1.13, 95 % CI: 1.00, 1.29) and non-Hispanic Blacks (RR=1.40, 95 % CI: 1.16, 1.68) experienced significantly higher mortality risk after exposure to UFPs, compared to non-Hispanic Whites. Children under five, older adults, non-NYC residents, and winter seasons are more susceptible to UFPs' effects.

Mysteriously rapid rise in Legionnaires' disease incidence correlates with declining atmospheric sulfur dioxide.

Legionnaires' disease (LD) is a severe form of pneumonia (∼10-25% fatality rate) caused by inhalation of aerosols containing Legionella, a pathogenic gram-negative bacteria. These bacteria can grow, spread, and aerosolize through building water systems. A recent dramatic increase in LD incidence has been observed globally, with a 9-fold increase in the United States from 2000 to 2018, and with disproportionately higher burden for socioeconomically vulnerable subgroups. Despite the focus of decades of research since the infamous 1976 outbreak, substantial knowledge gaps remain with regard to source of exposure and the reason(s) for the dramatic increase in LD incidence. Here, we rule out factors indicated in literature to contribute to its long-term increases and identify a hitherto unexplored explanatory factor. We also provide an epidemiological demonstration that the occurrence of LD is linked with exposure to cooling towers (CTs). Our results suggest that declining sulfur dioxide air pollution, which has many well-established health benefits, results in reduced acidity of aerosols emitted from CTs, which may prolong the survival duration of Legionella in contaminated CT droplets and contribute to the increase in LD incidence. Mechanistically associating decreasing aerosol acidity with this respiratory disease has implications for better understanding its transmission, predicting future risks, and informed design of preventive and interventional strategies that consider the complex impacts of continued sulfur dioxide changes.

The importance of ammonia for springtime atmospheric new particle formation and aerosol number abundance over the United States.

New particle formation (NPF) and subsequent growth can contribute upwards of 50 % of the global cloud condensation nuclei (CCN) budget. It is also a significant source of ultrafine aerosols (PM0.1) with health implications. Ammonia (NH3) can play a significant role in enhancing NPF and contributing to the growth of nucleated particles. Understanding these processes are vital for air quality and climate. Here, we examine the role of NH3 in NPF and consequent effects on aerosol number concentrations (including CCN) and size distributions during springtime over the United States (US). We use the GEOS-Chem chemistry transport model coupled with the size-resolved Advanced Particle Microphysics (APM) Model. We also employ measurements of particle number size distributions, CN10 (condensation nuclei > 10 nm), CCN0.4 (CCN at 0.4 % supersaturation), and aerosol composition (SO4, NO3, NH4, Organics) at the Southern Great Plains site (SGP). The impact of NH3 in ion-mediated nucleation is the improved capturing of the occurrence of almost all springtime (March-April) NPF events observed at SGP during 2015-2020. Furthermore, this brings the magnitude and temporal variations of particle number concentrations in stronger agreement with observations; mean fractional bias for modeled CN10(CCN0.4) reducing from -1.26 to -0.27 (-0.75 to -0.54) and overall good-agreement (∣FractionalBias ∣ < 0.6) improving from 8.5 to 54 % (31 to 42 %). The contribution of NH3 in new particle formation is important for springtime abundance of ultrafine aerosols (explaining 63 ± 15 % of CN10) and CCN (16 ± 10 % of CCN0.4) over the US. Our analysis shows that the deviation of CCN0.4 is strongly correlated with PM1-NH4+ deviations, suggesting the importance of improved model representation of ammonium for more accurate quantification of potential cloud forming particles.

The independent and synergistic impacts of power outages and floods on hospital admissions for multiple diseases.

Highly destructive disasters such as floods and power outages (PO) are becoming more commonplace in the U.S. Few studies examine the effects of floods and PO on health, and no studies examine the synergistic effects of PO and floods, which are increasingly co-occurring events. We examined the independent and synergistic impacts of PO and floods on cardiovascular diseases, chronic respiratory diseases, respiratory infections, and food-/water-borne diseases (FWBD) in New York State (NYS) from 2002 to 2018. We obtained hospitalization data from the NYS discharge database, PO data from the NYS Department of Public Service, and floods events from NOAA. Distributed lag nonlinear models were used to evaluate the PO/floods-health association while controlling for time-varying confounders. We identified significant increased health risks associated with both the independent effects from PO and floods, and their synergistic effects. Generally, the Rate Ratios (RRs) for the co-occurrence of PO and floods were the highest, followed by PO alone, and then floods alone, especially when PO coverage is >75th percentile of its distribution (1.72% PO coverage). For PO and floods combined, immediate effects (lag 0) were observed for chronic respiratory diseases (RR:1.58, 95%CI: 1.24, 2.00) and FWBD (RR:3.02, 95%CI: 1.60, 5.69), but delayed effects were found for cardiovascular diseases (lag 3, RR:1.13, 95%CI: 1.03, 1.24) and respiratory infections (lag 6, RR:1.85, 95%CI: 1.35, 2.53). The risk association was slightly stronger among females, whites, older adults, and uninsured people but not statistically significant. Improving power system resiliency could be a very effective way to alleviate the burden on hospitals during co-occurring floods. We conclude that PO and floods have independently and jointly led to increased hospitalization for multiple diseases, and more research is needed to confirm our findings.

Particle surface area, ultrafine particle number concentration, and cardiovascular hospitalizations.

While the health impacts of larger particulate matter, such as PM10 and PM2.5, have been studied extensively, research regarding ultrafine particles (UFPs or PM0.1) and particle surface area concentration (PSC) is lacking. This case-crossover study assessed the associations between exposure to PSC and UFP number concentration (UFPnc) and hospital admissions for cardiovascular diseases (CVDs) in New York State (NYS), 2013-2018. We used a time-stratified case-crossover design to compare the PSC and UFPnc levels between hospitalization days and control days (similar days without admissions) for each CVD case. We utilized NYS hospital discharge data to identify all CVD cases who resided in NYS. UFP simulation data from GEOS-Chem-APM, a state-of-the-art chemical transport model, was used to define PSC and UFPnc. Using a multi-pollutant model and conditional logistic regression, we assessed excess risk (ER)% per inter-quartile change of PSC and UFPnc after controlling for meteorological factors, co-pollutants, and time-varying variables. We found immediate and lasting associations between PSC and overall CVDs (lag0-lag0-6: ERs% (95% CI%) ranges: 0.4 (0.1,0.7) - 0.9 (0.7-1.2), and delayed and prolonged ERs%: 0.1-0.3 (95% CIs: 0.1-0.5) between UFPnc and CVDs (lag0-3-lag0-6). Exposure to larger PSC was associated with immediate ER increases in stroke, hypertension, and ischemic heart diseases (1.1%, 0.7%, 0.8%, respectively, all p < 0.05). The adverse effects of PSC on CVDs were highest among children (5-17 years old), in the fall and winter, and during cold temperatures. In conclusion, we found an immediate, lasting effects of PSC on overall CVDs and a delayed, prolonged impact of UFPnc. PSC was a more sensitive indicator than UFPnc. The PSC effects were higher among certain CVD subtypes, in children, in certain seasons, and during cold days. Further studies are needed to validate our findings and evaluate the long-term effects.

Long-Term Trend of Gaseous Ammonia Over the United States: Modeling and Comparison With Observations.

The concentrations of atmospheric ammonia ([NH3]) have been observed to be increasing over the United States in the last decade, especially in Eastern United States. It is important to understand this temporal trend and variation due to the role of NH3 in particle formation and its ecological effects. Here the long-term trend of [NH3] over the United States is investigated using GEOS-Chem, a global 3-D tropospheric chemistry model, and is corroborated with empirical evidence from the Ammonia Monitoring Network. Model simulations, consistent with observations, show increase in [NH3] over the United States from 2001 to 2016, with magnitude largest in the East (~5% to 12%/year) and smallest in the West (~0% to 5%/year). Reasons for this are examined, and evidence for the role of decreasing SO2 and NOx emissions in increasing [NH3] is provided. The contributions of meteorology and NH3 emission changes to the [NH3] increase appear to be small during the period. Our sensitivity study suggests that decreasing SO2 and NOx emissions over the United States owing to stringent regulations explain about 2/3 and 1/3 of the increase in [NH3], respectively. This effect is different for various NH3 and SO2 and NOx regimes. Given the continued reduction of SO2 and NOx emissions due to U.S. regulations mainly aimed at PM2.5 reduction, the present results are important towards better assessing the environmental impact of emission controlling policies.