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1.
ACS Earth Space Chem ; 7(3): 653-660, 2023 Mar 16.
Article in English | MEDLINE | ID: mdl-36960424

ABSTRACT

Aerosol nucleation accounts for over half of all seed particles for cloud droplet formation. In the atmosphere, sulfuric acid (SA) nucleates with ammonia, amines, oxidized organics, and many more compounds to form particles. Studies have also shown that methanesulfonic acid (MSA) nucleates independently with amines and ammonia. MSA and SA are produced simultaneously via dimethyl sulfide oxidation in the marine atmosphere. However, limited knowledge exists on how MSA and SA nucleate together in the presence of various atmospherically relevant base compounds, which is critical to predicting marine nucleation rates accurately. This work provides experimental evidence that SA and MSA react to form particles with amines and that the SA-MSA-base nucleation has different reaction pathways than SA-base nucleation. Specifically, the formation of the SA-MSA heterodimer creates more energetically favorable pathways for SA-MSA-methylamine nucleation and an enhancement of nucleation rates. However, SA-trimethylamine nucleation is suppressed by MSA, likely due to the steric hindrance of the MSA and trimethylamine. These results display the importance of including nucleation reactions between SA, MSA, and various amines to predict particle nucleation rates in the marine atmosphere.

2.
J Phys Chem A ; 126(44): 8240-8248, 2022 Nov 10.
Article in English | MEDLINE | ID: mdl-36287779

ABSTRACT

Atmospheric nucleation from precursor gases is a significant source of cloud condensation nuclei in the troposphere and thus can affect the Earth's radiative balance. Sulfuric acid, ammonia, and amines have been identified as key nucleation precursors in the atmosphere. Studies have also shown that atmospheric ions can react with sulfuric acid to form stable clusters in a process referred to as ion-induced nucleation (IIN). IIN follows similar reaction pathways as chemical ionization, which is used to detect and measure nucleation precursors via atmospheric pressure chemical ionization mass spectrometers. The rate at which ions form clusters depends on the ion-molecule rate constant. However, the rate constant varies based on the ion composition, which is often not known in the atmosphere. Previous studies have examined ion-molecule rate constants for sulfuric acid and nitrate ions but not for other atmospherically relevant ions like acetate. We report the relative rate constants of ion-molecule reactions between nitrate and acetate ions reacting with sulfuric acid. The ion-molecule rate constant for acetate and sulfuric acid is estimated to be a factor of 1.9-2.4 times higher than that of the known rate constant for nitrate and sulfuric acid. Using quantum chemistry, we find that acetate has a higher dipole moment and polarizability than nitrate. This may contribute to an increase in the collision cross-sectional area between acetate and sulfuric acid and lead to a greater reaction rate constant than nitrate. The ion-molecule rate constant for acetate with sulfuric acid will help quantify the contribution of acetate ions to atmospheric ion-induced new particle formation.

3.
PLoS One ; 17(9): e0273194, 2022.
Article in English | MEDLINE | ID: mdl-36137079

ABSTRACT

Severe viral respiratory diseases, such as SARS-CoV-2, are transmitted through aerosol particles produced by coughing, talking, and breathing. Medical procedures including tracheal intubation, extubation, dental work, and any procedure involving close contact with a patient's airways can increase exposure to infectious aerosol particles. This presents a significant risk for viral exposure of nearby healthcare workers during and following patient care. Previous studies have examined the effectiveness of plastic enclosures for trapping aerosol particles and protecting health-care workers. However, many of these enclosures are expensive or are burdensome for healthcare workers to work with. In this study, a low-cost plastic enclosure was designed to reduce aerosol spread and viral transmission during medical procedures, while also alleviating issues found in the design and use of other medical enclosures to contain aerosols. This enclosure is fabricated from clear polycarbonate for maximum visibility. A large single-side cutout provides health care providers with ease of access to the patient with a separate cutout for equipment access. A survey of medical providers in a local hospital network demonstrated their approval of the enclosure's ease of use and design. The enclosure with appropriate plastic covers reduced total escaped particle number concentrations (diameter > 0.01 µm) by over 93% at 8 cm away from all openings. Concentration decay experiments indicated that the enclosure without active suction should be left on the patient for 15-20 minutes following a tracheal manipulation to allow sufficient time for >90% of aerosol particles to settle upon interior surfaces. This decreases to 5 minutes when 30 LPM suction is applied. This enclosure is an inexpensive, easily implemented additional layer of protection that can be used to help contain infectious or otherwise potentially hazardous aerosol particles while providing access into the enclosure.


Subject(s)
COVID-19 , Infectious Disease Transmission, Patient-to-Professional , Aerosolized Particles and Droplets , COVID-19/prevention & control , Humans , Infectious Disease Transmission, Patient-to-Professional/prevention & control , Plastics , Respiratory Aerosols and Droplets , SARS-CoV-2
4.
J Phys Chem A ; 126(25): 4057-4067, 2022 Jun 30.
Article in English | MEDLINE | ID: mdl-35729723

ABSTRACT

Alkanolamines such as monoethanolamine (MEA), diethanolamine (DEA), and triethanolamine (TEA) are extensively used for CO2 capture and consumer products. Despite their prevalence in industrial applications, the fate of alkanolamines in the atmosphere remains relatively unknown. One likely reaction pathway for these chemicals in the atmosphere is new particle formation with sulfuric acid. Here, we present the first experimental results showing the formation of sulfuric acid dimers enhanced by MEA, DEA, and TEA from the measurement of molecular clusters. This study examines the nucleation reactions of MEA, DEA, and TEA with sulfuric acid in a clean, laminar flow reactor. The chemical compositions and concentrations of the freshly nucleated clusters were analyzed using a custom-built atmospheric pressure chemical ionization long time-of-flight mass spectrometer known as the Pittsburgh Cluster CIMS. Quantum chemical calculations and kinetic modeling of sulfuric acid-MEA/DEA/TEA clusters were also performed to determine relative cluster stabilities between these sulfuric acid-base systems. Experimental results indicate that MEA, DEA, and TEA at the part per trillion by volume (pptv) concentrations can enhance sulfuric acid dimer formation rates but to a lesser extent than dimethylamine (DMA). Thus, MEA, DEA, and TEA will potentially play an important role in new particle formation in industrial cities where these alkanolamines are emitted.


Subject(s)
Ethanolamine , Sulfuric Acids , Atmosphere/chemistry , Ethanolamine/chemistry , Models, Theoretical , Sulfuric Acids/chemistry
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