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Using a coated-insert flow tube reactor coupled to a low-energy electron-impact mass spectrometer with molecular beam sampling, we studied uptake of NO3 by sea salt at room temperature and [NO3]?=?8?1011???4?1013 molecule cm?3. The radical uptake coefficient γ(t) is time dependent: its initial value (γ ini) decreases exponentially with the characteristic time (τ) to its steady-state value (γ ss) at given [NO3]. The parameters γ ini, γ ss and τ depend on [NO3], whereas γ ss is water vapor independent at [H2O]?=?8?1012???1.6?1015 molecule cm?3 and RH ≤ 0.5 %. HCl and NO2 are uptake products detected in the gas phase. We used these findings to estimate γ values under tropospheric conditions for urban coastal and remote marine environments: at high NO3 (~90 ppt), the time dependence becomes important, and the γ value averaged over the aerosol lifetime is 4?10?3; at low NO3 (~1 ppt), the radical uptake is time independent and proceeds faster with γ ini?=?8?10?3  相似文献   
2.
A simple kinetic mechanism of nitrate radicals uptake on dry sea-salt NaCl, NaBr surfaces is proposed. The mechanism includes adsorption/desorption equilibrium and unimolecular decomposition of the adsorbed complex: NO3(g) + NaX(s) (NO3-NaX)(s); (NO3-NaX)(s) NaNO3 + X(s) Two techniques were used: the matrix isolation ESR and mass spectrometry. The uptake coefficient () is found to be dependent on exposure time of salt to NO3 for raw coating. The initial (t0) is higher than the observable steady-state obs. At room temperature obs is independent of [NO3] at low [NO3] = 3 × 109 - 1011 cm-3, but it is inversely proportional to [NO3] at concentrations higher than 1012 cm-3. At temperatures above 100 °C, obs becomes independent of [NO3] in a wider range of [NO3]. An increased number of dislocations is supposed to exist in the case of raw coating. Due to a wide spread of the surface sites binding energy with the ionic lattice near dislocations, the part of surface complexes has lower binding energy and "burns" more rapidly. That burning determines the transition from (t0) down to obs.The kinetic parameters and elementary rate coefficients are obtained. The recommended for low atmospheric NO3 concentration are in the range of 0.002 ± 0.04 for NaCl and 0.1-0.3 for NaBr depending on a mechanism of the (t) relaxation.  相似文献   
3.
Oceanology - The results of research carried out on cruise 62 of the R/V Akademik Oparin from December 14 to 29, 2020 continued monitoring of the interannual variability of the Japan Sea water...  相似文献   
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