Citation: WANG Tian-He, LIU Ze, WANG Wei-Gang, GE Mao-Fa. Heterogeneous Uptake Kinetics of Limonene and Limonene Oxide by Sulfuric Acid Solutions[J]. Acta Physico-Chimica Sinica, ;2012, 28(07): 1608-1614. doi: 10.3866/PKU.WHXB201204241 shu

Heterogeneous Uptake Kinetics of Limonene and Limonene Oxide by Sulfuric Acid Solutions

WANG Tian-He ^1,2 ,
LIU Ze ¹ ,
WANG Wei-Gang ^1, ,
GE Mao-Fa ^1,

1.
1. State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China;
2. Graduate University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Received Date: 26 March 2012
Available Online: 24 April 2012
Fund Project: 国家重点基础研究发展规划项目(973) (2011CB403401) (973) (2011CB403401)国家自然科学基金(40925016, 21077109, 41005070)资助 (40925016, 21077109, 41005070)

The heterogeneous uptake of limonene and limonene oxide (also known as 1,8-cineole) by a range of different aqueous sulfuric acid (H₂SO₄) solutions (30%-80% (w)) was investigated to develop an understanding of the reactivity of biogenic organic compounds in the atmosphere towards acidic aerosols. Experiments were performed using a rotating wetted-wall reactor coupled to a single photon ionization time-of-flight mass spectrometer. The heterogeneous uptake of the compounds into H₂SO₄ followed first-order kinetics and the corresponding steady-state uptake coefficients (γ) were calculated for the first time. Limonene oxide was found to be more reactive than limonene towards H₂SO₄. Reactive uptake was observed for limonene oxide in acidic solution containing greater than 30% (w). The steady-state uptake coefficients of limonene oxide in 30%-50% (w) H₂SO₄ solutions at room temperature ranged from (7.100± 0.023)×10^-5 to (8.150±0.162)×10^-3. Furthermore, the reactions of limonene oxide with sulfuric acid in bulk solution were investigated using gas chromatography-mass spectrometry (GC-MS) and electron spray ionization-mass spectroscopy (ESI-MS). Analysis of the products revealed the presence of monoterpenes, terpineols, terpin hydrates, and terpin hydrate diorganosulfate from the bulk solution reaction of limonene oxide with H₂SO₄. The formation of significantly more hydrophobic organic compounds with lower volatilities suggested that limonene oxide is a significant precursor in the formation of atmospheric secondary organic aerosols. A transformation mechanism has been proposed based on the products.
- Limonene,
- Limonene oxide,
- Sulfuric acid,
- Heterogeneous kinetics,
- Steady-state uptake coefficient,
- Organosulfate
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