Nucleation of particles with sulfuric acid, water, and nitrogeneous bases was studied in a flow reactor. Sulfuric acid and water levels were set by flows over sulfuric acid and water reservoirs, respectively, and the base concentrations were determined from measured permeation rates and flow dilution ratios. Particle number distributions were measured with a nano-differential-mobility-analyzer system. Results indicate that the nucleation capability of NH 3 , methylamine, dimethylamine, and trimethylamine with sulfuric acid increases from NH 3 as the weakest, methylamine next, and dimethylamine and trimethylamine the strongest. Three other bases were studied, and experiments with triethylamine showed that it is less effective than methylamine, and experiments with urea and acetamide showed that their capabilities are much lower than the amines with acetamide having basically no effect. When both NH 3 and an amine were present, nucleation was more strongly enhanced than with just the amine present. Comparisons of nucleation rates to predictions and previous experimental work are discussed, and the sulfuric acid-base nucleation rates measured here are extrapolated to atmospheric conditions. The measurements suggest that atmospheric nucleation rates are significantly affected by synergistic interactions between ammonia and amines.
Nucleation of particles composed of sulfuric acid, water, and nitrogen base molecules was studied using a continuous flow reactor. The particles formed from these vapors were detected with an ultrafine condensation particle counter, while vapors of sulfuric acid and nitrogen bases were detected by chemical ionization mass spectrometry. Variation of particle numbers with sulfuric acid concentration yielded a power dependency on sulfuric acid of 5 ± 1 for relative humidities of 14–68% at 296 K; similar experiments with varying water content yielded power dependencies on H<sub>2</sub>O of ~7. The critical cluster contains about 5 H<sub>2</sub>SO<sub>4</sub> molecules and a new treatment of the power dependency for H<sub>2</sub>O suggests about 12 H<sub>2</sub>O molecules for these conditions. Addition of 2-to-45 pptv of ammonia or methyl amine resulted in up to millions of times more particles than in the absence of these compounds. Particle detection capabilities, sulfuric acid and nitrogen base detection, wall losses, and the extent of particle growth are discussed. Results are compared to previous laboratory nucleation studies and they are also discussed in terms of atmospheric nucleation scenarios
Nucleation of particles composed of sulfuric acid, water, and nitrogen base molecules was studied using a continuous flow reactor. The particles formed from these vapors were detected with an ultrafine condensation particle counter, while vapors of sulfuric acid and nitrogen bases were detected by chemical ionization mass spectrometry. Variation of particle numbers with sulfuric acid concentration yielded a power dependency on sulfuric acid of 5 ± 1 for relative humidities of 14–68% at 296 K; similar experiments with varying water content yielded power dependencies on H<sub>2</sub>O of ~7. The critical cluster contains about 5 H<sub>2</sub>SO<sub>4</sub> molecules and a new treatment of the power dependency for H<sub>2</sub>O suggests about 12 H<sub>2</sub>O molecules for these conditions. Addition of 2-to-45 pptv of ammonia or methyl amine resulted in up to millions of times more particles than in the absence of these compounds. Particle detection efficiencies, sulfuric acid and nitrogen base detection, wall losses, and the extent of particle growth are discussed with the help of a recent computational fluid dynamics study that simulated the flow and chemistry in the flow reactor. Results are compared to previous laboratory nucleation studies and they are also discussed in terms of atmospheric nucleation scenarios
Particle formation and growth with H(2)SO(4) molecules in an axially symmetric flow reactor was simulated with computational fluid dynamics. A warm (~310 K) gas containing H(2)SO(4) flows into a cooled section (296 K) that induces particle formation. The fluid dynamics gives flow fields, temperatures, and reactant and cluster distributions. Particle formation and growth are simulated with detailed H(2)SO(4) cluster kinetics with chemistry based on measured small cluster thermodynamics and on bulk thermodynamics for large clusters. Results show that particle number densities have power law dependencies on sulfuric acid of ~7, in accord with the thermodynamics of the cluster chemistry. The region where particle formation rates are largest has a temperature that is within 3 K of the wall. Additional simulations show that the H(2)SO(4) concentration in this region is 5 to 10 times greater than the measured H(2)SO(4): this information allows for direct comparisons of experiment and theory. Experiments where ammonia was added as a third nucleating species were simulated with a three-dimensional model. Ammonia was dispersed quickly and particle formation during this mixing was seen to be low. Downstream of the initial mixing region, however, ammonia greatly affected particle formation.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
customersupport@researchsolutions.com
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
This site is protected by reCAPTCHA and the Google Privacy Policy and Terms of Service apply.
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.