| Autor: |
Fomete SKW; Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.; Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States., Johnson JS; Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.; Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States., Myllys N; Department of Chemistry, University of Jyväskylä, P.O. Box 35, FI-40014 Jyväskylä, Finland., Jen CN; Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.; Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States. |
| Abstrakt: |
Alkanolamines such as monoethanolamine (MEA), diethanolamine (DEA), and triethanolamine (TEA) are extensively used for CO 2 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. |
