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1.
Isoprene peroxy radical isomerizations (1,5- and 1,6-H shifts) have recently been proposed as important pathways regenerating and recycling HOx (OH?+?HO2) in the atmosphere under low-NOx conditions (Peeters et al. Phys. Chem. Chem. Phys. 28: 5935?C5939 2009; da Silva et al. Environ. Sci. Technol. 44:250?C256 2010). Evaluation and comparison of the isoprene peroxy radical isomerization mechanisms from recent studies have been performed against isoprene-NOx experiments conducted in the UNC dual outdoor smog chambers. Five different kinetic mechanisms were tested in this study, including the original Master Chemical Mechanism (MCM) v3.1; two modified MCM mechanisms both implementing isoprene peroxy radical isomerization reactions but with different rate coefficients; the Carbon Bond 6 (CB6) mechanism; and the ISO-UNC mechanism. Sensitivity analyses of the unsaturated hydroxyperoxy aldehydes (HPALDs) reaction mechanisms under fast isomerization have also been performed. The results indicate that the fast isomerization mechanism and the mechanisms with high OH yields from HPALDs photolysis both significantly enhance HOx estimates with increasing isoprene/NOx ratios. However, O3 predictions, as well the isoprene decay rates are substantially overestimated. Our results suggest that given the current state of our knowledge, it is difficult to improve both HOx levels and maintain reasonable O3 simulations using the Peeters et al. (Peeters et al. Phys. Chem. Chem. Phys. 28: 5935?C5939 2009) mechanism.  相似文献   

2.
The representation of alkene degradation in version 3 of the Master Chemical Mechanism (MCM v3) has been evaluated, using environmental chamber data on the photo-oxidation of ethene, propene, 1-butene and 1-hexene in the presence of NOx, from up to five chambers at the Statewide Air Pollution Research Center (SAPRC) at the University of California. As part of this evaluation, it was necessary to include a representation of the reactions of the alkenes with O(3P), which are significant under chamber conditions but generally insignificant under atmospheric conditions. The simulations for the ethene and propene systems, in particular, were found to be sensitive to the branching ratios assigned to molecular and free radical forming pathways of the O(3P) reactions, with the extent of radical formation required for proper fitting of the model to the chamber data being substantially lower than the reported consensus. With this constraint, the MCM v3 mechanisms for ethene and propene generally performed well. The sensitivity of the simulations to the parameters applied to a series of other radical sources and sink reactions (radical formation from the alkene ozonolysis reactions and product carbonyl photolysis; radical removal from the reaction of OH with NO2 and β-hydroxynitrate formation) were also considered, and the implications of these results are discussed. Evaluation of the MCM v3 1-butene and 1-hexene degradation mechanisms, using a more limited dataset from only one chamber, was found to be inconclusive. The results of sensitivity studies demonstrate that it is impossible to reconcile the simulated and observed formation of ozone in these systems for ranges of parameter values which can currently be justified on the basis of the literature. As a result of this work, gaps and uncertainties in the kinetic, mechanistic and chamber database are identified and discussed, in relation to both tropospheric chemistry and chemistry important under chamber conditions which may compromise the evaluation procedure, and recommendations are made for future experimental studies. Throughout the study, the performance of the MCM v3 chemistry was also simultaneously compared with that of the corresponding chemistry in the SAPRC-99 mechanism, which was developed and optimized in conjunction with the chamber datasets.  相似文献   

3.
Using the “lumped mechanism” and “counting species” methods, we developed a condensed gas-phase chemical model based on a simplified one. The modified quasi-steady-state approximation (QSSA) scheme and the error redistribution mass conservation technique are adopted to solve the atmospheric chemistry ki-netic equations. Results show that the condensed model can well simulate concentration variations of gas species such as SO2, NOx, O3, H2O2 and conversion rates of SO2 and NOx, transformation to H2SO4 and HNO3. These results are in good agreement with those from the simplified model, The conversion rates of SO2 and NOx under different initial concentrations and meteorological conditions are computed, and the results can be directly applied to regional acid deposition model.  相似文献   

4.
大气化学机理的发展及应用   总被引：3，自引：0，他引：3  
大气化学机理是研究大气化学过程的重要手段和方法之一,也是发展空气质量模式必不可少的重要组成部分。作者综述了几种应用广泛的简化机理——碳键机理（Carbon Bond Mechanism,CBM）、加州大气污染研究中心机理（Statewide Air Pollution Research Center mechanism,SAPRC）、区域酸沉降机理（Regional Acid Deposition Mechanism,RADM）、区域大气化学机理（Regional Atmospheric Chemical Mechanism,RACM）以及详细化学机理——主要大气化学机理（Master Chemical Mechanism,MCM）和共同代表性中间体机理（Common Representative Intermediates,CRI）的发展及应用。对上述大气化学机理的产生、发展、包含的物种类型、集总方式等方面进行了对比分析,总结了采用烟雾箱数据评价大气化学机理的研究成果以及大气化学机理在模式发展方面的应用,并对大气化学机理的进一步发展与完善提出了需求。  相似文献   

5.
Measurements of total peroxy radicals (HO2?+?RO2) and nitrate radical (NO3) were made on the NOAA research vessel R/V?Brown along the U.S. Gulf Coast during the TexAQS 2006 field campaign. The measurements were modelled using a constrained box-model based upon the Master Chemical Mechanism (MCM). The agreement between modelled and measured HO2?+?RO2 was typically within ??40% and, in the unpolluted regions, within 30%. The analysis of the model results suggests that the MCM might underestimate the concentrations of some acyl peroxy radicals and other small peroxy radicals. The model underestimated the measurements of NO3 by 60?C70%, possibly because of rapid heterogeneous uptake of N2O5. The MCM model results were used to estimate the composition of the peroxy radical pool and to quantify the role of DMS, isoprene and alkenes in the formation of RO2 in the different regions. The measurements of HO2?+?RO2 and NO3 were also used to calculate the gas-phase budget of NO3 and quantify the importance of organic peroxy radicals as NO3 sinks. RO2 accounted, on average, for 12?C28% of the total gas-phase NO3 losses in the unpolluted regions and for 1?C2% of the total gas-phase NO3 losses in the polluted regions.  相似文献   

6.
Emissions of biogenic volatile organic compounds (BVOC) were measured using a relaxed eddy accumulation (REA) technique on an above-canopy tower in a temperate forest (Changbai Mountain, Jilin province, China) during the 2010 and 2011 summer seasons. Solar global radiation and photosynthetically active radiation (PAR) were also measured. Based on PAR energy dynamic balance, an empirical BVOC emission and PAR transfer model was developed that includes the processes of BVOC emissions and PAR transfer above the canopy level, including PAR absorption and consumption, and scattering by gases, liquids, and particles (GLPs). Simulated emissions of isoprene and monoterpenes were in agreement with observations. The averages of the relative estimator biases for the flux were 39.3 % for isoprene, and 27.1 % for monoterpenes in the 2010 and 2011 growing seasons, with NMSE (normalized mean square error) values of 0.133 and 0.101, respectively. The observed and simulated mean diurnal variations of isoprene and monoterpenes in the 2010 and 2011 growing seasons were evaluated for the validation of the empirical model. Under observed atmospheric conditions, the sensitivity analysis showed that emissions of isoprene and monoterpenes were more sensitive to changes in PAR than to water vapor content or to the magnitude of the scattering factor. The emissions of isoprene and monoterpenes in the 2010 and 2011 growing seasons (from June to September) were estimated using this empirical model along with hourly observational data, with mean hourly emissions of 1.71 and 1.55 mg m?2 h?1 for isoprene, and 0.48 and 0.47 mg m?2 h?1 for monoterpenes in 2010 and 2011, respectively. As formaldehyde (HCHO) is considered as the main oxidation product of isoprene and monoterpenes, it is necessary to investigate the link between HCHO and BVOC emissions. GOME-2 HCHO vertical column densities (VCDs) can be used to estimate BVOC emission fluxes in the Changbai Mountain temperate forest.  相似文献   

7.
Greenhouse gas removal (GGR) approaches are considered essential in several projections to meet the climate mitigation ambition of the Paris Agreement. Biomass Energy with Carbon Capture and Storage (BECCS) and afforestation are included extensively in mitigation scenarios but there are concerns about the feasibility of these approaches. This was explored with stakeholders from industry, non-governmental organisations (NGOs) and policy who were involved in interviews and a one-day participatory workshop. Multicriteria mapping (MCM) methodology was used to appraise the ‘real-world’ feasibility of four specific greenhouse gas removal supply chains at a granular level in the UK context. The MCM analysis shows that afforestation performs better in comparison to three BECCS supply chains, on criteria such as business model, social acceptability, and environmental sustainability. This innovative application of the MCM methodology enables the abstract representations of GGR in integrated assessment models to be explored at a more granular level through a supply chain analysis and thus gain a deeper understanding of the issues facing these approaches. The data gathered allows a wide range of technical, environmental, social and political criteria to be systematically applied in appraising the practical performance of different future implementation options for afforestation and BECCS. If these GGR supply chains are to become a reality on the scale required for 1.5 °C global warming, factors such as global cooperation, land availability, and the longevity of policies and incentives were found to be major challenges.  相似文献   

8.
Compared to other phytoplankton groups, nitrogen-fixing cyanobacteria generally prefer high water temperatures for growth and are therefore expected to benefit from global warming. We use a coupled biological-physical model with an advanced cyanobacteria life cycle model to compare the abundance of cyanobacteria in the Baltic Sea during two different time periods (1969–1998; 2069–2098). For the latter, we find prolonged growth and a more than twofold increase in the climatologically (30 years) averaged cyanobacteria biomass and nitrogen fixation. Additional sensitivity experiments indicate that the biological-physical feedback mechanism through light absorption becomes more important with global warming. In general, we find a nonlinear response of cyanobacteria to changes in the atmospheric forcing fields as a result of life-cycle related feedback mechanisms. Overall, the sensitivity of the cyanobacteria-driven system suggests that biological-physical and life-cycle related feedback mechanisms are important and must therefore be included in future projection studies.  相似文献   

9.
正The atmospheric oxidation capacity(AOC) is the essential driving force of atmospheric chemistry in forming complex air pollution, which determines the removal rate of trace gases and the production rates of secondary pollutants. The processes and rates of species being oxidized in the atmosphere thus constitute the key factors to quantify the AOC. Currently,  相似文献   

10.
A three-dimensional Lagrangian tropospheric chemistry modelis used toinvestigate the impact of human activities on the tropospheric distributionofozone and hydroxyl radicals. The model describes the behaviour of 50 speciesincluding methane, carbon monoxide, oxides of nitrogen, sulphur dioxide andnineorganic compounds emitted from human activities and a range of other sources.Thechemical mechanism involves about 100 chemical reactions of which 16 arephotochemical reactions whose diurnal dependence is treated in full. The modelutilises a five minute chemistry time step and a three hour advection timestepfor the 50,000 air parcels. Meteorological data for the winds, temperatures,clouds and so on are taken from the UK Meteorological Office global model for1994 onwards. The impacts of a 50% reduction in European NOXemissions onglobal ozone concentrations are assessed. Surface ozoneconcentrations decrease in summertime and rise in wintertime, but to differentextents.  相似文献   

11.
Although a large volume of monitoring and computer simulation data exist for global coverage of HF, study of HF in the troposphere is still limited to industry whose primary interest is the safety and risk assessment of HF release because it is a toxic gas. There is very limited information on atmospheric chemistry, emission sources, and the behavior of HF in the environment. We provide a comprehensive review on the atmospheric chemistry of HF, modeling the reactions and transport of HF in the atmosphere, the removal processes in the vertical layer immediately adjacent to the surface (up to approximately 500 m) and recommend research needed to improve our understanding of atmospheric chemistry of HF in the troposphere. The atmospheric chemistry, emissions, and surface boundary layer transport of hydrogen fluoride (HF) are summarized. Although HF is known to be chemically reactive and highly soluble, both factors affect transport and removal in the atmosphere, the chemistry can be ignored when the HF concentration is at a sufficiently low level (e.g., 10 ppmv). At a low concentration, the capability for HF to react in the atmosphere is diminished and therefore the species can be mathematically treated as inert during the transport. At a sufficiently high concentration of HF (e.g., kg/s release rate and thousands of ppm), however, HF can go through a series of rigorous chemical reactions including polymerization, depolymerization, and reaction with water to form molecular complex. As such, the HF species cannot be considered as inert because the reactions could intimately influence the plume’s thermodynamic properties affecting the changes in plume temperature and density. The atmospheric residence time of HF was found to be less than four (4) days, and deposition (i.e., atmosphere to surface transport) is the dominant mechanism that controls the removal of HF and its oligomers from the atmosphere. The literature data on HF dry deposition velocity was relatively high compared to many commonly found atmospheric species such as ozone, sulfur dioxide, nitrogen oxides, etc. The global average of wet deposition velocity of HF was found to be zero based on one literature source. Uptake of HF by rain drops is limited by the acidity of the rain drops, and atmospheric particulate matter contributes negligibly to HF uptake. Finally, given that the reactivity of HF at a high release rate and elevated mole concentration cannot be ignored, it is important to incorporate the reaction chemistry in the near-field dispersion close to the proximity of the release source, and to incorporate the deposition mechanism in the far-field dispersion away from the release source. In other words, a hybrid computational scheme may be needed to address transport and atmospheric chemistry of HF in a range of applications. The model uncertainty will be limited by the precision of boundary layer parameterization and ability to accurately model the atmospheric turbulence.  相似文献   

12.
Mechanism reductions of the detailed aqueous phase chemistry mechanism CAPRAM 3.0i are performed. Manual methods and automatic techniques are both applied in order to provide a less computationally intensive mechanism which is operational in regional chemistry transport models (CTMs). The finally reduced mechanism contains less than 200 reactions (4 times smaller than the detailed CAPRAM 3.0i) and describes the main characteristics of inorganic and organic aqueous phase processes occurring in tropospheric warm clouds. Most of the chemical reduction potential is realized in the CAPRAM 3.0i organic chemistry. The number of aqueous phase species decreases from 380 in the full mechanism to 130 in the final reduced version. The calculated percentage deviations between the full and reduced mechanism are on average below 5% for the most important organic and inorganic target compounds such as oxidants, inorganic and organic acids, carbonyls and alcohols. Comparisons of the required CPU times between the full and reduced mechanisms show reductions of approximately 40%. 2-D test simulations with the CTM MUSCAT were performed using prescribed meteorological conditions in order to examine the applicability of the reduced mechanism at regional scale. Simulations with the reduced CAPRAM 3.0i mechanism and a much less complex mechanism with only limited inorganic chemistry (INORG) were compared to evaluate the effects of more detailed chemistry. The model results show large differences in the level of oxidants and the inorganic and organic mass processing. Prospectively, the reduced mechanism represents the basis for studying aerosol cloud processing effects at regional scale with future CTMs and will allow more adequate interpretation of field data.  相似文献   

13.
The regional climate model (RegCM3) and a tropospheric atmosphere chemistry model (TACM) were coupled, thus a regional climate chemistry modeling system (RegCCMS) was constructed, which was applied to investigate the spatial distribution of anthropogenic nitrate aerosols, indirect radiative forcing, as well as its climatic effect over China. TACM includes the thermodynamic equilibrium model ISORROPIA and a condensed gas-phase chemistry model. Investigations show that the concentration of nitrate aerosols is relatively high over North and East China with a maximum of 29 μg m-3 in January and 8 μg m-3 in July. Due to the influence of air temperature on thermodynamic equilibrium, wet scavenging of precipitation and the monsoon climate, there are obvious seasonal differences in nitrate concentrations. The average indirect radiative forcing at the tropopause due to nitrate aerosols is -1.63 W m-2 in January and -2.65 W m-2 in July, respectively. In some areas, indirect radiative forcing reaches $-$10 W m-2. Sensitivity tests show that nitrate aerosols make the surface air temperature drop and the precipitation reduce on the national level. The mean changes in surface air temperature and precipitation are -0.13 K and -0.01 mm d-1 in January and -0.09 K and -0.11 mm d-1 in July, respectively, showing significant differences in different regions.  相似文献   

14.
The laser flash photolysis/UV absorption spectrometry technique has been used to investigate the kinetics of the peroxy radical permutation reactions (i.e. self and cross reactions) arising from the OH-initiated oxidation of isoprene (2-methyl-1,3-butadiene), and of the simpler, but related conjugated dienes, 1,3-butadiene and 2,3-dimethyl-1,3-butadiene. The results of the two simpler systems are analysed to provide values of the rate coefficients for the 6 peroxy radical permutation reactions of the three types of isomeric peroxy radical produced in each system (T = 298 K, P = 760 Torr). The rate coefficients are all significantly larger than values estimated previously by extrapolation of structure-reactivity relationships based on the kinetics of a limited dataset of simpler radicals containing similar structural features. The results are discussed in terms of trends in self and cross reaction reactivity of primary, secondary and tertiary peroxy radicals containing combinations of allyl, -hydroxy and -hydroxy functionalities. Since the peroxy radicals formed in these systems are structurally very similar to those formed in the isoprene system, the kinetic parameters derived from the results of the simpler systems are used to assist the assignment of kinetic parameters to the 21 permutation reactions of the six types of isomeric peroxy radical generated in the isoprene system. Kinetic models describing the OH-initiated degradation of all three conjugated dienes to first generation products in the absence of NOx are recommended, which are also consistent with available end product studies. The model for isoprene is considered to be a further improvement on that suggested previously for its OH-initiated oxidation in the absence of NOx. The mechanism is further extended to include chemistry applicable to NOx-present conditions, and calculated product yields are compared with those reported in the literature.  相似文献   

15.
Global secondary organic aerosol formation (SOA) is currently assumed to be between 11.2 and 270 Tg/yr. This range of uncertainty is reflected in the gas-phase chemistry. In this study, we focus on the feedback of SOA formation on the concentrations of most important trace gases such as ozone, and compare it to the impact of monoterpene gas-phase chemistry with a newly developed reduced monoterpene mechanism (MMM) for either α- or β-pinene in the global chemistry transport model MATCH-MPIC. With this set-up an uncertainty range of 3.5–4.0% increase in annually averaged tropospheric ozone was found to be caused by the gas-phase chemistry of the investigated monoterpenes. Moreover, a strong feedback has been observed for NOx, HCHO, HNO3 and PAN. These observations are affected remarkably by different SOA formation approaches like partitioning or saturation vapour pressure limitation and by the structure of the monoterpene used, e.g. reducing the impact on tropospheric ozone to 1.2–1.9% by using the partitioning approach versus the simulation with gas-phase chemistry only. Therefore, a consideration of the individual processes associated with SOA formation seems to be necessary to reduce the uncertainty in SOA formation and to understand the impact of VOCs on atmospheric chemistry. An erratum to this article is available at .  相似文献   

16.
Autoxidation of S(IV) initiated by manganese sulphate or potassium peroxydisulphate in alkaline aqueous solutions was significantly slowed down by dissolved isoprene, which decayed in the process. The laboratory experiments were carried out in a batch, perfectly mixed reactor, which had no gas space. The concentration–time profiles of oxygen were measured with a Clark-type electrode. The profiles of sulphite species and of isoprene were evaluated from the UV spectra of solutions. The kinetic analysis indicated that isoprene reacted directly with sulphate radical anions produced during the S(IV) autoxidation. A relative second-order rate constant of (2.12 ± 0.37) × 109 M–1 s–1 was determined for this reaction at 25 °C, pH (8.0–8.5) and ionic strength of (1.7–4.9) × 10–3 M (the reference rate constant of the reaction of sulphate radical anions with sulphite ions equalled 3.4 × 108 M–1 s–1). A tentative mechanism of isoprene oxidation during S(IV) autoxidation, which included formation of isoprene – SO– 4 adduct, was based on the analogy to the gas-phase reactions of isoprene and to the liquid-phase reactions of sulphate radical anions with other compounds. Atmospheric significance of the aqueous-phase reaction of isoprene with sulphate radicals was discussed. Approximate analysis showed the reaction is a potential sink for isoprene in the aqueous phase and in the gas–liquid systems of high liquid water content (LWC > 10–5 m3 m–3). The aqueous-phase oxidation of isoprene can produce secondary pollutants, and influence transformation and the long-range transport of SO2 in the atmosphere.  相似文献   

17.
In this study, an improved and complete secondary organic aerosols (SOA) chemistry scheme was implemented in the CHIMERE model. The implementation of isoprene chemistry for SOA significantly improves agreement between long series of simulated and observed particulate matter concentrations. While simulated organic carbon concentrations are clearly improved at elevated sites by adding the SOA scheme, time correlation are impaired at low level sites in Portugal, Italy and Slovakia. At several sites a clear underestimation by the CHIMERE model is noticed in wintertime possibly due to missing wood burning emissions as shown in previous modeling studies. In Europe, the CHIMERE model gives yearly average SOA concentrations ranging from 0.5 μg m  − 3 in the Northern Europe to 4 μg m  − 3 over forested regions in Spain, France, Germany and Italy. In addition, our work suggests that during the highest fire emission periods, fires can be the dominant source of primary organic carbon over the Mediterranean Basin, but the SOA contribution from fire emissions is low. Isoprene chemistry has a strong impact on SOA formation when using current available kinetic schemes.  相似文献   

18.
We present a theory for the formation of frozen aerosol particles in the Antarctic stratosphere, the coldest region of the Earth's stratosphere. The theory is applied specifically to the formation of polar stratospheric clouds. We suggest that the condensed ices are composed primarily of nitric acid and water with small admixtures of other compounds such as H2SO4 and HCl in solid solution. Our assumed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinctions observed in the winter polar stratosphere. Physical chemistry and thermodynamic considerations suggest that at temperatures between about 200 and 185 K, stratospheric particulates are composed primarily of frozen nitric acid solutions with a composition near that of the trihydrate. Available data suggest the particles are amorphous solid solutions and not in the crystalline hydrate form. At lower temperatures (i.e., below the forst point of pure water) cirrus-like ice clouds can form.  相似文献   

19.
地球系统模式是研究全球气候与生态环境变化问题的重要工具，气溶胶与大气化学模式负责为其中的大气环流模式提供与气候效应有关的气态化学物质和气溶胶成分。本文在全球嵌套网格空气质量预报模式系统的基础上发展了一个适用于中国科学院地球系统模式（CAS-ESM）耦合计算的气溶胶与大气化学分量模式（IAP-AACM），采用简化的气相化学机制，不仅考虑了人为气溶胶，同时考虑了海盐、沙尘和二甲基硫等自然气溶胶及其前体物的在线排放。评估结果表明，IAP-AACM氧化剂插值计算可靠，采用简化机制和碳键机制（CBM-Z）模拟的差异较小。和观测的对比表明，得益于CAS-ESM的气溶胶双向反馈作用，简化版能够较好地抓住气溶胶及其前体物的空间分布，为IAP-AGCM提供可靠的气溶胶模拟。另外，简化版能大幅提升计算效率，满足CAS-ESM耦合长期积分的需求。为了在全球气候变化的研究中提供更完善的气溶胶模拟，未来考虑在IAP-AACM中增加氮化学和臭氧平流层化学机制。  相似文献   

20.
Two recent gas-phase chemical kinetic mechanisms for tropospheric ozone formation, one based on the lumped-structure approach (CB05) and the other based on the lumped-molecule approach (RACM2), are compared for simulations of ozone over Europe. The host air quality model is POLAIR3D of the Polyphemus modeling platform. A one-month period (15 July to 15 August 2001) is simulated. Model performance is satisfactory with both mechanisms. Overall, the two mechanisms give similar results with a domain-averaged difference of 3 ppb and a mean fractional absolute difference of 5% (values averaged over the month for the daily 8-h average maximum ozone concentrations). This difference results from different treatments in the two mechanisms for both inorganic and organic chemistry. Differences in the treatment of the inorganic chemistry are due mainly to differences in the kinetics of two reactions: NO + O3 \(\longrightarrow\) NO2 + O2 and NO + HO2 \(\longrightarrow\) NO2 + OH. These differences lead to a domain-averaged difference in ozone concentration of 5%, with RACM2 kinetics being more conducive to ozone formation. Differences in the treatment of organic chemistry lead to a domain-averaged difference in ozone concentration of 3%, with CB05 chemistry being more conducive to ozone formation. This average difference results in part from compensating effects among various VOC classes and some significant differences are identified at specific locations (the coastline of northern Africa and eastern Europe: 9%) and for specific organic classes (aldehydes, biogenic alkenes and aromatics). Differences in the treatment of the organic chemistry result from various aspects. For some VOC classes, such as aldehydes and biogenic alkenes, the more detailed explicit treatments using more model species in RACM2 lead to either greater or lower reactivity depending on the assumptions made for the oxidation products. For other VOC species, such as aromatics, the assumptions made about the major chemical oxidation pathways (aromatic alcohol formation in CB05 vs. ring opening in RACM2) affect the ozone formation significantly. Reconciliation of different chemical kinetic mechanisms will require experimental data to reduce current uncertainties in the kinetic (e.g., NO oxidation) and mechanistic (e.g., aromatics oxidation) representations of major chemical pathways.  相似文献   

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