In this thesis, a new aerosol module is developed for the STEM model (the Sulfur Transport and dEposition Model) to better understand the chemical aging of dust during long range transport and assess the impact of heterogeneous reactions on tropospheric chemistry. The new aerosol module is verified and first applied in a box model, and then coupled into the 3-Dimentional STEM model. In the new aerosol model, a non-equilibrium (dynamic or kinetic) approach to treat gas-to-particular conversion is employed to replace the equilibrium method in STEM model. Meanwhile, a new numerical method solving the aerosol dynamics equation is introduced into the dynamic aerosol model for its improved computational efficiency and high accuracy. Compared with the equilibrium method, the new dynamic approach is found to provide better results on predicating the different hygroscopicity and chemical aging patterns as a function of size. The current modeling study also takes advantage of new findings from laboratory experiments about heterogeneous reactions on mineral oxides and dust particles, in order to consider the complexity of surface chemistry (such as surface saturation, coating and relative humidity). Modeling results show that the impacts of mineralogy and relative humidity on heterogeneous reactions are significant and should be considered in atmospheric chemistry modeling with first priority. Finally, the upgraded 3-D STEM model is utilized to explore the observations from the Intercontinental Chemical Transport Experiment - Phase B (INTEX-B). The new dynamic approach for gas-to-particular conversion and RH-dependent heterogeneous uptake of HNO3 improve the model performance in term of aerosol predictions under different conditions. It is shown that these improvements change the modeled nitrate and sulfate concentrations, but also modify their size distributions significantly.
Dissertation
Modeling the effects of heterogeneous reactions on atmospheric chemistry and aerosol properties
University of Iowa
Doctor of Philosophy (PhD), University of Iowa
Autumn 2010
DOI: 10.17077/etd.2xewzpnz
Free to read and download, Open Access
Abstract
Details
- Title: Subtitle
- Modeling the effects of heterogeneous reactions on atmospheric chemistry and aerosol properties
- Creators
- Chao Wei - University of Iowa
- Contributors
- Gregory R. Carmichael (Advisor)Vicki H. Grassian (Committee Member)Charles O. Stanier (Committee Member)David G. Rethwisch (Committee Member)Thomas M. Peters (Committee Member)
- Resource Type
- Dissertation
- Degree Awarded
- Doctor of Philosophy (PhD), University of Iowa
- Degree in
- Chemical and Biochemical Engineering
- Date degree season
- Autumn 2010
- Publisher
- University of Iowa
- DOI
- 10.17077/etd.2xewzpnz
- Number of pages
- x, 106 pages
- Copyright
- Copyright 2010 Chao Wei
- Language
- English
- Description bibliographic
- Includes bibliographical references (pages 100-106).
- Academic Unit
- Chemical and Biochemical Engineering
- Record Identifier
- 9983777251502771
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