Environmental Aerosol Research Articles

Photooxidation of Nonanoic Acid by Molecular and Complex Environmental Photosensitizers.

Photochemical aging and photooxidation of atmospheric particles play a crucial role in both the chemical and physical processes occurring in the troposphere. In particular, the presence of organic chromophores within atmospheric aerosols can trigger photosensitized oxidation that drives the atmospheric processes in these interfaces. However, the light-induced oxidation of the surface of atmospheric aerosols, especially those enriched with organic components, remains poorly understood. Herein, we present a gravimetric and vibrational spectroscopy study aimed to investigate the photosensitized oxidation of nonanoic acid (NA), a model system of fatty acids within organic aerosols, in the presence of complex organic photosensitizers and molecular proxies. Specifically, this study shows a comparative analysis of the photosensitized reactions of thin films containing nonanoic acid and four different organic photosensitizers, namely marine dissolved organic matter (m-DOM) and humic acids (HA) as environmental photosensitizers, and 4-imidazolecarboxaldehyde (4IC) and 4-benzoylbenzoic acid (4BBA) as molecular proxies. All reactions show predominant photooxidation of nonanoic acid, with important differences in the rate and yield of product formation depending on the photosensitizer. Limited changes were observed in the organic photosensitizer itself. Results show that, among the photosensitizers examined, 4BBA is the most effective in photooxidizing nonanoic acid. Overall, this work underscores the role of chromophores in the photooxidation of organic thin films and the relevance of such reactions on the surface of aerosols in the marine environment.

Covalent Self-Assembly of Bio-HCP Nanoparticles for Shell-Programmed Encapsulation of Microbial Cells.

Modifying the bacterial surface through grafting functional nanoparticles is a common strategy for programing bacteria. At this moment, the targeted nanoparticles face a dilemma of no multifunctional structure, high toxicity, and weak chemical driving forces, which restrict the broad practical applications. Like a multistage booster of a rocket, we propose a multistage covalent self-assembly strategy to protect, expand, and control the encapsulated shells of microbial cells via biocompatible hyper-cross-linked polymer nanoparticles (Bio-HCP NPs) with internal porosity and surface functional groups. The bacterial surface is enhanced with rich amino groups up to 1010 per cell for specifically grafting nanoparticles. The arming bacteria after first-stage assembly can complete biocatalysis in a highly toxic environment, and as-prepared polymer aggregates (6-20 μm) after third-stage assembly can be accurately counted in an aerosol environment. This nanoparticle encapsulation exhibits strong cell viability from pollutants and specificity from impurity particles, holding promise for various complex application scenarios.

Composition and Biogeochemical Effects of Carbohydrates in Aerosols in Coastal Environment

We adopted a simple and rapid measurement method to analyze the concentrations of monosaccharides (MCHO) and polysaccharides (PCHO) in carbohydrates, a subset of organic carbon found in size-fractionated atmospheric particles. Seasonal and source-related factors influenced carbohydrate concentrations, with total water-soluble carbohydrates (TCHO) accounting for approximately 23% of the water-soluble organic carbon (WSOC) in spring when biological activity was high. We observed that the mode of aerosol transport significantly influenced the particle size distribution of carbohydrates, with MCHO exhibiting relatively high concentrations in fine particles (<1 μm) and PCHO showing higher concentrations in coarse particles (>1 μm). Moreover, our results revealed that MCHO and PCHO contributed 51% and 49%, respectively, to the TCHO concentration. This contribution varied by approximately ±19% depending on the season, suggesting the importance of both MCHO and PCHO. Additionally, through the combined use of principal component analysis (PCA) and positive matrix factorization (PMF), we determined that biomass burning accounts for 30% of the aerosol. Notably, biomass burning accounts for approximately 52% of the WSOC flux, with MCHO accounting for approximately 78% of the carbon from this source, indicating the substantial influence of biomass burning on aerosol composition. The average concentration of TCHO/WSOC in the atmosphere was approximately 18%, similar to the marine environment, reflecting the relationship between the biogeochemical cycles of the two environments. Finally, the fluxes of MCHO and PCHO were 1.10 and 5.28 mg C m−2 yr−1, respectively. We also found that the contribution of atmospheric deposition to marine primary productivity in winter was 15 times greater than that in summer, indicating that atmospheric deposition had a significant impact on marine ecosystems during nutrient-poor seasons. Additionally, we discovered that WSOC accounts for approximately 62% of the dissolved organic carbon (DOC) in the Min River, suggesting that atmospheric deposition could be a major source of organic carbon in the region.

Influence of different cleaning methods on the concentration of airborne endotoxins and microbial aerosols in the oral clinical environment

AimThis study aims to evaluate the effectiveness of various cleaning methods in reducing airborne endotoxin and microbial aerosols during oral cleaning procedures.MethodForty patients undergoing oral cleaning procedures were randomly assigned to one of four groups (n = 10 per group). Group A received strong suction alone; Group B received strong suction combined with an air disinfection machine; Group C received strong suction combined with a dental electric suction machine; Group D received strong suction in conjunction with both an air disinfection machine and a dental electric suction machine. Airborne aerosol concentrations were assessed at four-time points: before treatment, 30 min into treatment, immediately after treatment, and 60 min after treatment ended. Samples were collected at distances of 20 cm, 60 cm, and 1 m from the patient’s oral cavity using the natural sedimentation method. T-test was used to evaluate the difference among tested groups.ResultsAirborne endotoxins and microbial aerosols levels increased significantly during treatment, with the highest levels observed at 20 cm from the patient’s mouth. During treatment, groups with additional cleaning methods (Groups B, C, and D) exhibited higher levels of airborne endotoxins and microbial aerosols compared to Group A (strong suction alone). However, post-treatment analysis revealed that Group D demonstrated the lowest level of airborne endotoxins and microbial aerosols, while Group A exhibited the highest.ConclusionsImplementing effective aerosol management strategies can significantly reduce aerosol dispersion in the oral clinical environment. Continuous monitoring aerosol concentrations and the application of appropriate control measures are essential for minimizing infection risks for both patients and healthcare providers during oral cleaning procedures.

A novel “cells-on-particles” cytotoxicity testing platform in vitro: design, characterization, and validation against engineered nanoparticle aerosol

The presented research introduces the "Cells-on-Particles" integrated aerosol sampling and cytotoxicity testing in vitro platform, which allows for the direct assessment of the biological effects of captured aerosol particles on a selected cell type without the need for extraction or resuspension steps. By utilizing particles with unaltered chemical and physical properties, the method enables simple and fast screening of biological effects on specific cell types, making it a promising tool for assessing the cytotoxicity of particulate matter in ambient and occupational air. Platforms fabricated from cellulose acetate (CA) and poly[ε]caprolactone (PCL) were proven to be biocompatible and promoted the attachment and growth of the human bronchial epithelial cell line BEAS-2B. The PCL platforms were exposed to simulated occupational aerosols of silver, copper, and graphene oxide nanoparticles. Each nanoparticle type exhibited different and dose-dependent cytotoxic effects on cells, evidenced by reduced cell viability and distinct, particle type-dependent gene expression patterns. Notably, copper nanoparticles were identified as the most cytotoxic, and graphene oxide the least. Comparing the “Cells-on-Particles" and submerged exposure (“Particles-on-Cells") testing strategies, BEAS-2B cells responded to selected nanoparticles in a comparable manner, suggesting the developed testing system could be proposed for further evaluation with more complex environmental aerosols. Despite limitations, including particle agglomeration and the need for more replicates to address variability, the “Cells-on-Particles” platform enables effective detection of toxicity induced by relatively low levels of nanoparticles, demonstrating good sensitivity and a relatively simpler procedure compared to standard 2D cell exposure methods.

Pathogen shape: Implication on pathogenicity via respiratory deposition

The shape of environmental aerosols contributes to the discrepancy in their dynamic behavior compared to spherical particles, which have received inadequate consideration. We reported deposition patterns of aerosols and aerosol-transmissible pathogens in real human respiratory systems, taking into account their actual shape, using a validated computational-based model. We found that the shape of the aerosols significantly influenced its deposits and accessibility within the respiratory system, significantly in the tracheobronchial region. As an example, we estimated that over 180 % of differences in deposits in the trachea and bronchi were attributable to pathogens shape, inferring the underlying pathogenicity difference of these regions. These findings, capturing the spatial heterogeneity of pathogens and aerosols deposition in human respiratory system, have major implication for understanding the evolution of aerosol-related disease.

Influence of bulk-phase acidity, organic fraction, and dissolved oxygen on the photosensitized renoxification of nitrate in NaNO3/humic acid mixtures

Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets. Although numerous nitrite acid (HONO) formation pathways from nitrate photolysis have been widely reported, the influence of various environmental factors and aerosol properties on reactive nitrogen production remains largely unclear. In this work, we employed NaNO3/humic acid (HA) as a model nitrate photosensitization system to investigate the crucial roles of aerosol acidity, organic fraction, and dissolved oxygen in the production of HONO, NO2, and NO2-. The presence of HA at 10 mg/L resulted in a remarkable increase in HONO production rates by approximately 2–3 times and NO2- concentration by 3–6 times across a pH range of 5.2 to 2.0. Meanwhile, the molar fraction of gaseous HONO in total N(III) production increased from 4 % to 69 % as bulk-phase pH decreased from 5.2 to 2.0. The higher organic fraction (i.e., 20 and 50 mg/L HA concentration) instead inhibited HONO and NO2 release. The presence of dissolved oxygen was found to be adverse for reactive nitrogen production. This suggests that the HA photosensitizer promoted the secondary conversion of NO2 to HONO mainly via reduced ketyl radical intermediates, while superoxide radical formation might exert a negative effect. Our findings provide comprehensive insights into reactive nitrogen production from photosensitized nitrate photolysis mediated by various external and internal factors, potentially accounting for discrepancies between field observations and model simulations.

Temporal variation characteristics of microbial aerosols in the goose house environment

ABSTRACT 1. Preventing disease is important in poultry production systems, but this has mainly been studied in chickens. The aim of this study is to explore the impact of microbial aerosols in intensive goose house environments. 2. To evaluate the environmental quality of geese housing, fine particulate matter (PM2.5) was collected using an ambient air particulate matter sampler. High-throughput sequencing was used to analyse bacterial diversity and relative abundance. Results showed that the number of general and operational taxonomic units (OTUs) were 1,578 and 19 112 in all PM2.5 samples. Firmicutes, Bacteroidota, Proteobacteria, Acidobacterota were the four most abundant phyla in PM2.5. 3. Compared with bacterial phyla in the PM2.5 from chicken houses, those in the genus Acidobacterota were increased in goose housing. There are various genera of bacteria present in PM2.5, and their composition was similar across different samples. No significant change was observed in the diversity of microbiota in the PM2.5, although multiple pathogenic bacteria were detected. 4. A prediction function showed that a variety of bacterial phyla correlated positively with the human diseases. 5. In summary, the microbial aerosols in the goose shed pose significant risks to the health of the geese. Regular monitoring of the composition of microbial aerosols is important for the healthy growth of geese and disease prevention and control.

Spatial distribution of bioaerosols and evaluation of four ventilation method on controlling their diffusion in a typical enhanced biosafety level 2 laboratory

Biosafety laboratories are critical in many fields. However, experimenters associated the infection risk from biological aerosols. In this study, by conducting experiments on the release and collection of bioaerosols within a typical BSL-2 + laboratory, the spatial distribution of bioaerosols was tracked. Numerical calculations were employed to obtain and visualize the airflow patterns and aerosol dispersion paths of four ventilation methods. The results indicated that equipment and tables led to uneven airflow distribution within the laboratory. The comparison results of the four evaluation indicators showed that the air age distribution of UU (Upward supply and upward return) mode and CD (Cross-supply and downward return) mode was superior, with air change efficiency values of 0.595 and 0.603, respectively. Additionally, the contaminant removal index of CD mode was 1.48, significantly higher than the other ventilation methods. The statistical results of the contaminant dispersion index also indicated that CD mode was most conducive to diluting aerosols in the spatial environment. The LD (lateral supply and downward return) mode may lead to airflow short-circuiting. The UD (upward supply and downward return) mode can provide balanced protection for laboratory. Overall, CD mode performed the best among the four ventilation methods, followed by UU mode.

Intercomparison of aerosol optical depths from four reanalyses and their multi-reanalysis consensus

Abstract. The emergence of aerosol reanalyses in recent years has facilitated a comprehensive and systematic evaluation of aerosol optical depth (AOD) trends and attribution over multi-decadal timescales. Notable multi-year aerosol reanalyses currently available include NAAPS-RA from the US Naval Research Laboratory, the NASA MERRA-2, JRAero from the Japan Meteorological Agency (JMA), and CAMSRA from Copernicus/ECMWF. These aerosol reanalyses are based on differing underlying meteorology models, representations of aerosol processes, as well as data assimilation methods and treatment of AOD observations. This study presents the basic verification characteristics of these four reanalyses versus both AERONET and MODIS retrievals in monthly AOD properties and identifies the strength of each reanalysis and the regions where divergence and challenges are prominent. Regions with high pollution and often mixed fine-mode and coarse-mode aerosol environments, such as South Asia, East Asia, Southeast Asia, and the Maritime Continent, pose significant challenges, as indicated by higher monthly AOD root mean square error. Moreover, regions that are distant from major aerosol source areas, including the polar regions and remote oceans, exhibit large relative differences in speciated AODs and fine-mode versus coarse-mode AODs among the four reanalyses. To ensure consistency across the globe, a multi-reanalysis consensus (MRC, i.e., ensemble mean) approach was developed similarly to the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME). Like the ICAP-MME, while the MRC does not consistently rank first among the reanalyses for individual regions, it performs well by ranking first or second globally in AOD correlation and RMSE, making it a suitable candidate for climate studies that require robust and consistent assessments.

Research Note: The structure and diversity of antibiotic resistance genes in animal house environment

In recent years, a series of public health issues caused by the spread of antibiotic resistance have been widely concerned. The indoor air of livestock and poultry houses is considered to be one of the main sources of environmental contamination of ARGs. This study characterized the micro-organisms and ARGs in the air particulate matter of chicken houses using metagenomics. The study successfully detected 761 different subtypes of resistance genes including aminoglycosides, tetracyclines, MLSB etc., 4 types of mobile genetic elements, and various pathogenic microorganisms from the aerosols in the chicken coop environment. The results showed that the abundance of ARGs in the air of the chicken coop was at a relatively high level, correlation network analysis showed that multiple types of ARGs could promote the emergence of antibiotic-resistant bacteria.

Simulations of the impact of cloud condensation nuclei and ice-nucleating particles perturbations on the microphysics and radar reflectivity factor of stratiform mixed-phase clouds

Abstract. In this research, we delve into the influence of cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations on the morphology and abundance of ice particles in mixed-phase clouds, emphasizing the consequential impact of ice particle shape, number, and size on cloud dynamics and microphysics. Leveraging the synergy of the Advanced Microphysics Prediction System (AMPS) and the Kinematic Driver (KiD) model, we conducted simulations to capture cloud microphysics across diverse CCN and INP concentrations. The Passive and Active Microwave radiative TRAnsfer (PAMTRA) radar forward simulator further augmented our study, offering insights into how the concentrations of CCN and INPs affect radar reflectivities. Our experimental framework encompassed CCN concentrations ranging from 10 to 5000 cm−3 and INP concentrations from 0.001 to 10 L−1. Central to our findings is the observation that higher INP concentrations yield smaller ice particles, while an increase in CCN concentrations leads to a subtle growth in their dimensions. Consistent with existing literature, our results spotlight oblate-like crystals as dominant between temperatures of −20 and −16 °C. Notably, high-INP scenarios unveiled a significant prevalence of irregular polycrystals. The aspect ratio (AR) of ice particles exhibited a decline with the rise in both CCN and INP concentrations, highlighting the nuanced interrelation between CCN levels and ice particle shape, especially its ramifications on the riming mechanism. The forward-simulated radar reflectivities, spanning from −11.83 dBZ (low INP, 0.001 L−1) to 4.65 dBZ (high INP, 10 L−1), elucidate the complex dynamics between CCN and INPs in determining mixed-phase cloud characteristics. Comparable differences in radar reflectivity were also reported from observational studies of stratiform mixed-phase clouds in contrasting aerosol environments. Our meticulous analysis of KiD-AMPS simulation outputs, coupled with insights into aerosol-driven microphysical changes, thus underscores the significance of this study in refining our ability to understand and interpret observations and climate projections.

Inactivation Mechanisms of Escherichia coli in Simulants of Respiratory and Environmental Aerosol Droplets

The airborne transmission of disease relies on the ability of microbes to survive aerosol transport and, subsequently, cause infection when interacting with a host. The length of time airborne microorganisms remain infectious in aerosol droplets is a function of numerous variables. We present measurements of mass and heat transfer from liquid aerosol droplets combined with airborne survival data for Escherichia coli MRE162, an ACDP category 1 microorganism used as a model system, under a wide range of environmental conditions, droplet compositions and microbiological conditions. In tandem, these companion measurements demonstrate the importance of understanding the complex relationship between aerosol microphysics and microbe survival. Specifically, our data consist of the correlation of a wide range of physicochemical properties (e.g., evaporation rates, equilibrium water content, droplet morphology, compositional changes in droplet solute and gas phase, etc.), with airborne viability decay to infer the impact of aerosol microphysics on airborne bacterial survival. Thus, a mechanistic approach to support prediction of the survival of microorganisms in the aerosol phase as a function of biological, microphysical, environmental, and experimental (aerosol-generation and sampling) processes is presented. Specific findings include the following: surfactants do not increase bacteria stability in aerosol, while both the bacteria growth phase and bacteria concentration may affect the rate at which bacteria decay in aerosol.

The Role of Aqueous Solvation on the Intersystem Crossing of Nitrophenols.

The photochemistry of nitrophenols is a source of smog as nitrous acid is formed from their photolysis. Nevertheless, computational studies of the photochemistry of these widespread toxic molecules are scarce. In this work, the initial photodeactivation of ortho-nitrophenol and para-nitrophenol is modeled, both in gas phase and in aqueous solution to simulate atmospheric and aerosol environments. A large number of excited states, six for ortho-nitrophenol and 11 for para-nitrophenol, have been included and were all populated during the decay. Moreover, periodic time-dependent density functional theory (TDDFT) is used for both the explicitly included solvent and the solute. A comparison to periodic QM/MM (TDDFT/MM), with electrostatic embedding, is made, showing notable differences between the decays of solvated nitrophenols simulated with QM/MM and full (TD)DFT. A reduced intersystem crossing in aqueous solution could be observed thanks to the surface hopping approach using explicit, periodic TDDFT solvation including spin-orbit couplings.

A Molecular Approach for Detecting Bacteria and Fungi in Healthcare Environment Aerosols: A Systematic Review.

Molecular methods have become integral to microbiological research for microbial identification. This literature review focuses on the application of molecular methods in examining airborne bacteria and fungi in healthcare facilities. In January 2024, a comprehensive electronic search was carried out in esteemed databases including PubMed, Web of Science, and Scopus, employing carefully selected keywords such as ((bacteria) OR (virus) OR (fungi)) AND (aerosol) AND ((hospital) OR (healthcare) OR (dental office)) AND ((molecular) OR (PCR) OR (NGS) OR (RNA) OR (DNA) OR (metagenomic) OR (microarray)), following the PRISMA protocol. The review specifically targets healthcare environments with elevated concentrations of pathogenic bacteria. A total of 487 articles were initially identified, but only 13 met the inclusion criteria and were included in the review. The study disclosed that the prevalent molecular methodology for appraising aerosol quality encompassed the utilization of the PCR method, incorporating either 16S rRNA (bacteria) or 18S rRNA (fungi) amplification techniques. Notably, five diverse molecular techniques, specifically PFGE, DGGE, SBT, LAMP, and DNA hybridization methods, were implemented in five distinct studies. These molecular tests exhibited superior capabilities compared to traditional bacterial and fungal cultures, providing precise strain identification. Additionally, the molecular methods allowed the detection of gene sequences associated with antibiotic resistance. In conclusion, molecular testing offers significant advantages over classical microbiological culture, providing more comprehensive information.

A quanta-independent approach for the assessment of strategies to reduce the risk of airborne infection

The Wells-Riley model is extensively used for retrospective and prospective modelling of the risk of airborne transmission of infection in indoor spaces. It is also used when examining the efficacy of various removal and deactivation methods for airborne infectious aerosols in the indoor environment, which is crucial when selecting the most effective infection control technologies. The problem is that the large variation in viral load between individuals makes the Wells-Riley model output very sensitive to the input parameters and may yield a flawed prediction of risk. The absolute infection risk estimated with this model can range from nearly 0 % to 100 % depending on the viral load, even when all other factors, such as removal mechanisms and room geometry, remain unchanged. We therefore propose a novel method that removes this sensitivity to viral load. We define a quanta-independent maximum absolute before-after difference in infection risk that is independent of quanta factors like viral load, physical activity, or the dose-response relationships. The input data needed for a non-steady-state calculation are just the removal rates, room volume, and occupancy duration. Under steady-state conditions the approach provides an elegant solution that is only dependent on removal mechanisms before and after applying infection control measures. We applied this method to compare the impact of relative humidity, ventilation rate and its effectiveness, filtering efficiency, and the use of ultraviolet germicidal irradiation on the infection risk. The results demonstrate that the method provides a comprehensive understanding of the impact of infection control strategies on the risk of airborne infection, enabling rational decisions to be made regarding the most effective strategies in a specific context. The proposed method thus provides a practical tool for mitigation of airborne infection risk.

A Study on Accurate Ranging Method of a Dual-Wavelength Orthogonal FMCW Laser Fuze in a Complex Aerosol Environment

A Study on Accurate Ranging Method of a Dual-Wavelength Orthogonal FMCW Laser Fuze in a Complex Aerosol Environment

A Machine Learning Approach to Retrieving Aerosol Optical Depth Using Solar Radiation Measurements

Aerosol optical depth (AOD) constitutes a key parameter of aerosols, providing vital information for quantifying the aerosol burden and air quality at global and regional levels. This study demonstrates a machine learning strategy for retrieving AOD under cloud-free conditions based on the synergy of machine learning algorithms (MLAs) and ground-based solar irradiance data. The performance of the proposed methodology was investigated by applying different components of solar irradiance. In particular, the use of direct instead of global irradiance as a model feature led to better performance. The MLA-based AODs were compared to reference AERONET retrievals, which encompassed RMSE values between 0.01 and 0.15, regardless of the underlying climate and aerosol environments. Among the MLAs, artificial neural networks outperformed the other algorithms in terms of RMSE at 54% of the measurement sites. The overall performance of MLA-based AODs against AERONET revealed a high coefficient of determination (R2 = 0.97), MAE of 0.01, and RMSE of 0.02. Compared to satellite (MODIS) and reanalysis (MERRA-2 and CAMSRA) data, the MLA-AOD retrievals revealed the highest accuracy at all stations. The ML-AOD retrievals have the potential to expand and complement the AOD information in non-existing timeframes when solar irradiances are available.

Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics

Abstract. Adsorption and desorption of gases on liquid or solid substrates are involved in multiphase processes and heterogeneous chemical reactions. The desorption energy (Edes0), which depends on the intermolecular forces between adsorbate and substrate, determines the residence time of chemical species at interfaces. We show how Edes0 and temperature influence the net uptake or release of gas species, the rates of surface–bulk exchange and surface or bulk reactions, and the equilibration timescales of gas–particle partitioning. Using literature data, we derive a parameterization to estimate Edes0 for a wide range of chemical species based on the molecular mass, polarizability, and oxygen-to-carbon ratio of the desorbing species independent of substrate-specific properties, which is possible because of the dominant role of the desorbing species' properties. Correlations between Edes0 and the enthalpies of vaporization and solvation are rooted in molecular interactions. The relation between Edes0 and desorption kinetics reflects the key role of interfacial exchange in multiphase processes. For small molecules and semi-volatile organics (VOC, IVOC, SVOC), Edes0 values around 10–100 kJ mol−1 correspond to desorption lifetimes around nanoseconds to days at room temperature. Even higher values up to years are obtained at low temperatures and for low volatile organic compounds (LVOC, ELVOC/ULVOC) relevant for secondary organic aerosols (SOA). Implications are discussed for SOA formation, gas–particle partitioning, organic phase changes, and indoor surface chemistry. We expect these insights to advance the mechanistic and kinetic understanding of multiphase processes in atmospheric and environmental physical chemistry, aerosol science, materials science, and chemical engineering.

Consideration of environmental aerosols.

Consideration of environmental aerosols.