Global 3-D Model Analysis of TRACE-P HCN and CH3CN Measurements

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Global 3-D Model Analysis of TRACE-P HCN and CH3CN Measurements Qinbin Li, Daniel J. Jacob, Robert M. Yantosca Harvard Atmospheric Chemistry Modeling Group Hanwant B. Singh NASA Ames Research Center Makoto Koike University of Tokyo Glen W. Sachse NASA-Langley Research Center

Atmospheric Budget of HCN (pre-TRACE-P) Li et al. [2000] Total atmospheric burden (Tg N) 0.50 Atmospheric lifetime (months) 2.1-4.4 Sources (Tg N yr-1) Biomass burning 1.4-2.9 Sinks (Tg N yr-1) Ocean uptake 1.1-2.6 Oxidation by OH 0.3 Photolysis 0.2×10-2 Reaction with O(1D) 0.3×10-3 Biomass burning emission ratio (relative to CO): 1.1%.

Vertical profiles in marine background atmosphere: Evidence for oceanic uptake of HCN and CH3CN Background: CO < 120 ppbv, C2Cl4 < 10 pptv Inferred saturation ratios: 0.84 for HCN, 0.80 for CH3CN

CH3CN-HCN Correlation in TRACE-P Biomass burning “Shanghai plume” (flight 13) Biofuels (?) Red: C2Cl4 > 11 pptv Blue: C2Cl4 < 11 pptv

Use HCN/CO and CH3CN/CO ratios measured in Chinese pollution plumes to infer biofuel emission ratios Flight #13 Assuming fresh fossil fuel+biofuel emissions. CO: biofuel/(fossil fuel+biofuel) ~42% for Shanghai + Jiangsu + Zhejiang [D. Streets, 2001] . Hence HCN/CO biofuel emission ratio ~ 0.40%.

Correlations: > 2 km Emission ratios relative to CO (% molar): biomass burning Biofuel HCN 0.14 0.34 CH3CN 0.12 0.22 Asian CO emissions (March 2001): 14 Tg fossil fuel 13 Tg biofuel 59 Tg biomass burning

Simulated vs. observed vertical profiles Red: observation Blue: model Green: biomass burning Pink: biofuel Yellow (CO only): fossil fuel

Simulated vs. observed frequency distributions Red: observation Blue: model

Simulated vs. observed HCN columns Moshiri (44°N, 142°E) Rikubetsu (45°N, 144°E) Tsukuba (36°N, 140°E) Red: observation Blue: model

Atmospheric Budgets for HCN and CH3CN Li et al. [2000] in red HCN CH3CN Atmospheric burden (Tg N) 0.42 (0.50) 0.20 Atmospheric lifetime (month) 5.0 (2.1-4.4) 3.2 Sources (Tg N yr-1) Biomass burning 0.51 (1.4-2.9) 0.43 Biofuel 0.48 0.31 Sinks (Tg N yr-1) Ocean uptake 0.74 (1.1-2.6) 0.52 Oxidation by OH 0.25 (0.3) 0.22