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Global and regional impacts of HONO on the chemical composition of clouds and aerosols

机译:HONO对云和气溶胶化学成分的全球和区域影响

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摘要

Recently, realistic simulation of nitrous acid (HONO) based on theHONO / NO ratio of 0.02 was found to have a significant impact on theglobal budgets of HO (OH + HO) and gas phase oxidationproducts in polluted regions, especially in winter when other photolyticsources are of minor importance. It has been reported thatchemistry-transport models underestimate sulphate concentrations, mostlyduring winter. Here we show that simulating realistic HONO levels cansignificantly enhance aerosol sulphate (S(VI)) due to the increased formationof HSO. Even though in-cloud aqueous phase oxidation of dissolvedSO (S(IV)) is the main source of S(VI), it appears that HONO relatedenhancement of HO does not significantly affect sulphate becauseof the predominantly S(IV) limited conditions, except over eastern Asia.Nitrate is also increased via enhanced gaseous HNO formation andNO hydrolysis on aerosol particles. Ammonium nitrate is enhancedin ammonia-rich regions but not under ammonia-limited conditions.Furthermore, particle number concentrations are also higher, accompanied bythe transfer from hydrophobic to hydrophilic aerosol modes. This implies asignificant impact on the particle lifetime and cloud nucleating properties.The HONO induced enhancements of all species studied are relatively strong inwinter though negligible in summer. Simulating realistic HONO levels is foundto improve the model-measurement agreement of sulphate aerosols, mostapparent over the US. Our results underscore the importance of HONO for theatmospheric oxidizing capacity and corroborate the central role of cloudchemical processing in S(IV) formation.
机译:最近,发现基于0.02的HONO / NO比的逼真的亚硝酸(HONO)模拟对污染地区的HO(OH + HO)和气相氧化产物的全球预算有重大影响,特别是在冬季,当其他光解源为次要的。据报道,化学运输模型低估了硫酸盐浓度,主要是在冬季。在这里,我们表明,由于HSO的形成增加,模拟实际的HONO水平可以显着提高硫酸盐气溶胶(S(VI))。尽管溶解态SO(S(IV))的云内水相氧化是S(VI)的主要来源,但由于主要受S(IV)限制,除其他条件外,HONO的HO增强似乎并未显着影响硫酸盐。通过增加气态HNO的形成和气溶胶颗粒上NO的水解,硝酸盐含量也增加了。硝酸铵在富含氨的区域增强,但在不受氨限制的条件下并不增强。此外,颗粒数浓度也更高,伴随着从疏水气溶胶模式向亲水气溶胶模式的转移。这暗示了对粒子寿命和云成核特性的显着影响。HONO诱导的所有研究物种的增强在冬季都相对较强,尽管在夏季可以忽略不计。人们发现,模拟现实的HONO含量可以改善硫酸盐气溶胶的模型测量协议,这在美国最为明显。我们的结果强调了HONO对于大气氧化能力的重要性,并证实了云化学过程在S(IV)形成中的重要作用。

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