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Comparison of tropospheric gas-phase chemistry schemes for use within global models

机译:在全球模型中使用的对流层气相化学方案的比较

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Methane and ozone are two important climate gases with significanttropospheric chemistry. Within chemistry-climate and transport models thischemistry is simplified for computational expediency. We compare the stateof the art Master Chemical Mechanism (MCM) with six tropospheric chemistryschemes (CRI-reduced, GEOS-CHEM and a GEOS-CHEM adduct, MOZART-2, TOMCAT andCBM-IV) that could be used within composition transport models. We test theschemes within a box model framework under conditions derived from acomposition transport model and from field observations from a regionalscale pollution event. We find that CRI-reduced provides much skill insimulating the full chemistry, yet with greatly reduced complexity. We findsignificant variations between the other chemical schemes, and reach thefollowing conclusions. 1) The inclusion of a gas phaseN2O5+H2O reaction in one scheme and not others is a largesource of uncertainty in the inorganic chemistry. 2) There are significantvariations in the calculated concentration of PAN between the schemes, whichwill affect the long range transport of reactive nitrogen in global models.3) The representation of isoprene chemistry differs hugely between theschemes, leading to significant uncertainties on the impact of isoprene oncomposition. 4) Differences are found in NO3 concentrations in thenighttime chemistry. Resolving these four issues through furtherinvestigative laboratory studies will reduce the uncertainties within thechemical schemes of global tropospheric models.
机译:甲烷和臭氧是对流层化学性质很重要的两种重要的气候气体。在化学-气候和运输模型中,为便于计算,简化了该化学。我们将最先进的主要化学机理(MCM)与对流层化学方法(还原CRI,GEOS-CHEM和GEOS-CHEM加合物,MOZART-2,TOMCAT和CBM-IV)进行了比较。我们在框模型框架内的条件下,对这些化学反应进行了测试,这些条件是根据成分迁移模型和区域规模污染事件的实地观察得出的。我们发现,降低CRI可以提供许多模拟整个化学反应的技能,但大大降低了复杂性。我们发现其他化学方案之间存在显着差异,并得出以下结论。 1)一种方案而不是其他方案包含气相N 2 O 5 + H 2 O反应是该方案不确定性的主要来源无机化学。 2)两种方案之间PAN的计算浓度存在显着差异,这将影响全局模型中反应性氮的长距离传输.3)两种方案之间异戊二烯化学的表示差异很大,从而导致对异戊二烯对组成的影响存在重大不确定性。 4)夜间化学中NO 3 的浓度存在差异。通过进一步的研究性实验室研究解决这四个问题,将减少全球对流层模型化学方案中的不确定性。

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