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CAM3.0模式中黑碳及硫酸盐气溶胶浓度变化对东亚春季气候的影响研究.pdf 9页
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第31卷 第4期
气 象 科 学
Vo1．31．No．4
JournaloftheMeteorologicalSciences
Aug．，2011
胡海波，刘超，张媛，等．CAM3．0模式中黑碳及硫酸盐气溶胶浓度变化对东亚春季气候的影响研究．气象科学 ，)：
HU Haibo，LIU Chao，ZHANGYuan，eta1．TheeffectsofaerosolsinCAM3．0onclimateinEastAsiaduringborealspring
． Journal
oftheMeteorologicalSciences，)：466474．
CAM3．0模式 中黑碳及硫酸盐气溶胶浓度变化
对东亚春季气候的影响研究
(1南京大学大气科学学院灾害性天气气候研究所，南京210093
2南京信息工程大学大气科学学院，南京210093)
摘要 本文采用CAM3．0模式研究东亚地 区各种气溶胶浓度增加后对于东亚春季各气候要
素，尤其是对降水和春季风场的影响。在模式中通过分别对区域 (20～50。N，100～150。E)内黑碳
气溶胶浓度单独加倍、硫酸盐气溶胶浓度单独加倍、两种气溶胶浓度同时加倍的实验方法，探讨不
同气溶胶浓度变化在东亚春季气候变化中的具体作用。结果表明：在春季，3种气溶胶浓度增加方
式都使得东亚地区表现出降水中南部减少北部增加，低层大气西南风异常以及地面温度南部增加
北部减少。通过对 110～120。E的断面分析发现，硫酸盐与黑碳气溶胶在春季首先影响约800hPa
以上大气的温度并通过不同的动力机制影响东亚地区的风场，风场的改变进而导致了云量和降水
在东亚北方地区增多而中南部地区减少，并最终使得地面温度表现出东亚中南部地区增温而北方
地区相对降温的特征。
关键词 黑碳气溶胶；硫酸盐气溶胶；降水减少
分类号 461．8
文献标识码 A
TheeffectsofaerosolsinCAM 3．0on climatein
EastAsiaduringborealspring
ZHANG Yuan
JIANG Yiquan
(1SchoolofAtmosphericSciences，NanjingUniversity，Nanjing210093，China
2SchoolofAtmosphericSciences，NanjingUniversityofInformationScience&Technology，Nanjing210093，China)
Abstract Inthisstudy，weusedNCAR CAM3．0modeltostudytheclimateimpactsofincreasing
aerosolconcentration onEastAsiaclimateinbor
正在加载中，请稍后...海洋中云凝结核（CCN）
SULFATE AEROSOL GENERATION
SULFATE AEROSOL GENERATION
the MARINE ATMOSPHERE
generation of maritime cloud condensation nuclei (CCN) through
the ejection of jet and film droplets from bursting whitecap-produced
bubbles on the ocean surface has been well documented. The
processes involved in the transformation (evaporation and
crystallization) of these liquid droplets into their solid
form under varying conditions, however, has not previously
attracted much attention from atmospheric researchers.
set of laboratory investigations and field observations of
the characteristics, both physical and chemical, of seawater
droplets during phase change in a controlled environment have
revealed the following startling and very significant phenomena:
Characterization
of the ejected sulfate aerosols in comparison with field observation,
chemical processes inside the evaporating seawater droplets
and the mechanisms for the generation of secondary aerosols
in the marine atmosphere are presented with illustrations.
PLANT EMISSION
RAIN FORMATION
ECOLOGICAL
ATMOSPHERIC
CARBONACEOUS
POLLUTION CONTROL
A NEW MECHANISM for the GENERATION of
HIGH SULFATE ENRICHED AEROSOLS in the MARINE ATMOSPHERE
(CaSO/4, MgSO/4---NOT DMS)
Presented at: 9th WORLD CLEAN AIR CONGRESS
AUGUST 30- SEPTEMBER 4, 1992
MONTREAL, QUEBEC, CANADA上传用户：ubbcqvpdwg资料价格：5财富值&&『』文档下载 ：『』&&『』所属分类：机构：LASG基金：This study is supported by Project 8-1304 of IAP/CAS and Ninth-Five Key Project(96-908-01-06).分类号：X513文献出处：Acta Meteorologica Sinica 2001年04期关 键 词 ：&&&权力声明：若本站收录的文献无意侵犯了您的著作版权，请点击。摘要：正 With the data of complex refractive index of sulfate aerosol，the radiative properties of theaerosol under 8 relative humidity conditions are calculated in this paper。By using the concentrationdistribution from two CTM models and LASG GOALS/AGCM，the radiative forcing due tohygroscopic sulfate aerosol is simulated。The results show that(1)With the increase of relativehumidity，the mass extinction coefficiency factor decreases in the shortwave spectrum；singlescattering albedo keeps unchanged except for a little increase in longwave spectrum，andasymmetry factor increases in whole spectrum。(2)Larger differences occur in radiative forcingsimulated by using two CTM data，and the global mean forcing is—0。268 and—0。816 W/m~2，respectively。(3)When the impact of relative humidity on radiative property is taken into account，the distribution pattern of radiative forcing due to the wet particles is very similar to that of drysulfate，but the forcing value decreases by 60%。Abstract：正与硫酸盐气溶胶复折射指数的数据，本文计算了8相对湿度条件下气溶胶的辐射特性，利用两CTM模型和GOALS / AGCM的浓度分布，产生的辐射强迫tohygroscopic硫酸盐气溶胶模拟。结果表明：（1）随着相对湿度的增加，在短波频谱的质量消光系数系数降低；singlescattering反照率保持不变，除了在长波光谱略有增加，在整个频谱的非因素增加。（2）较大的差异发生在辐射forcingsimulated采用CTM数据，与全球平均强迫is-0.268 and-0.816 W /我~ 2，分别为。（3）当相对湿度对辐射特性的影响考虑在内，辐射强迫引起的湿颗粒的分布模式，drysulfate非常相似，但强迫值降低60%。正文快照：1 .INTRODUCTION Aerosols ean exert an influenee on the energy budget of atmosphere一earth system inboth direet and indireet ways.Beeause aerosols ean lead to a radiative foreing eomparablein magnitude but of opposite to rhat of greenhouse gases,mueh atte分享到：相关文献|Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols_文档库
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Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols
GEOPHYSICAL RESEARCH LETTERS, VOL. 33, L13808, doi:10.GL6
Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols
John Liggio 1and Shao-Meng Li 1
Received 2March 2006; revised 19May 2006; accepted 30May 2006; published 8July 2006.
[1]Organosulfates are observed in studies of pinonaldehyde reactions with acidic sulfate aerosols using aerosol mass spectrometry, during which a significant fraction of the pinonaldehyde reaction products were found to consist of organosulfate compounds that account for 6–51%of the initial SO =4mass. Resultant aerosol mass spectra were consistent with proposed sulfate ester mechanisms, which likely form stable products. The existence of organosulfates was also confirmed in studies of the reaction system in bulk solution. The formation of organosulfates suggests that conventional inorganic SO =4chemical analysis may underestimate total SO =mass in 4
ambient aerosols. Citation:Liggio, J., and S.-M. Li (2006),
Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols, Geophys. Res. Lett. , 33, L13808, doi:10.GL026079.
sulfate. Hence, evidence for covalently bound sulfate in aerosols is a key step in understanding this reaction pathway. A recent study has in fact reported organo-sulfates in ambient aerosols [Romero and Oehme , 2005].The present study strives to determine whether organo-sulfate formation occurs in aerosols, to elucidate reaction pathways, and to assess the importance of their formation as a heterogeneous mechanism. The uptake of pinonalde-hyde, a major semi-volatile product from a -pinene oxidation, on acidic SO 4aerosols, is used as a model process to demonstrate organosulfate formation and its implications with regard to SOA formation in the atmosphere.
2. Experiment
[4]The pinonaldehyde uptake experiments have been described by Liggio and Li [2006].Mono-dispersed aero-sols 310–360nm in diameter, consisting primarily of H 2SO 4but also (NH4) 2SO 4, were introduced into a 2m 3Teflon bag at a given relative humidity, followed by addition of gaseous pinonaldehyde. Aerosol inorganic and organic mass were quantified with an aerosol mass spec-trometer (AMS),which provided organic structural infor-mation [Jayne et al. , 2000].Seed aerosols were generated via liquid atomization followed by sizing with a differential mobility analyzer. The particle acidity was controlled by the H 2SO 4concentration in an (NH4) 2SO 4solution and by the RH in the chamber (3–65%),thus altering the HSO ?4to =
SO 4molar ratios (Table1).
[5]Pinonaldehyde vapor was introduced into the cham-ber via a zero air stream at 40°C passed through a spiked quartz filter and was measured by 2,4-DNPH scrubbing followed by off-line HPLC-UV analysis [Liggio and Li , 2006].Pinonaldehyde was synthesized via an oxidative bond cleavage of pinandiol [Glasius et al. , 1997]and was >90%pure.
[6]The pinonaldehyde reaction in a bulk sulfuric acid solution was studied to confirm the presence of sulfate esters. In each experiment 20m L of pinonaldehyde was spiked into a concentrated acid solution (0.9ml H 2SO 4, 0.1ml H 2O), followed by GC-MS analysis. An uncoated, deactivated fused silica column (0.25mm i.d., 5m) was used, which retains H 2SO 4for about 15min while other products elute immediately. In principle, once inorganic sulfate is removed from the sample matrix, sulfate esters can be confirmed by identifying fragments from the ioni-zation of organically bound SO 4(m/z48, 64, 80, 96) or its decomposition products (SO2). A 1m L injection of the reaction solution was analyzed with the GC injector heated to 250°C and a temperature program which began isother-mally at 60°C for 1min, followed by a ramp of 10°C min ?1
1. Introduction
[2]Organic compound nucleation and condensation are important pathways leading to secondary organic aerosols (SOA),which in turn have numerous global and local impacts. However, recent studies have now also implicated heterogeneous reactions as a route for SOA formation [Jang et al. , 2003; Kroll et al. , 2005].Such reactions may lead to a transformation of semi-volatile compounds to high molec-ular weight species or oligomers which can remain in aerosols, and are believed to arise via compounds contain-ing carbonyl functional groups, i.e., aldehydes and ketones. Indeed, some aldehydes and ketones, when exposed to seed aerosols, increase SOA yields, particularly on acidic aero-sols [Jang et al. , 2003].Potential reaction mechanisms include hydration, hemi-acetal and acetal formation, aldol condensation [Noziere and Riemer , 2003],and poly-merization [Jang and Kamens , 2001].Products resulting from these mechanisms have been identified by mass-spectrometric techniques in laboratory studies [Kalberer et al. , 2004].
[3]Whereas polymerization remained the focus of such studies, sulfate esters formed in the reaction with acidic sulfate have been largely unnoticed. This is partially due to difficulties detecting such species which may be somewhat non-volatile at typical GC injection temperatures, potentially thermally unstable, and not easily differentiated from inor-ganic sulfate. Mass spectra of sulfate esters from a complex aerosol matrix are likely ambiguous and easily confused with the spectra of other organic products or inorganic
Air Quality Research Division, Atmospheric Science &Technology Directorate, Science &Technology Branch, Environment Canada. Copyright 2006by the American Geophysical Union. /
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