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1.
应用初步建立的全球二维大气化学模式,对工业革命以来甲烷的长期变化进行了模拟研究。模式将CH4、CO和NOx排放源方案进行了参数化。在考虑了CH4排放源以及对OH浓度有重要影响的CO和NOx排放源的长期变化的基础上,模拟了CH4和OH浓度自1840年到20世纪90年代的长期变化趋势。结果表明,工业革命前的大气甲烷体积分数和年排放总量分别为760×10-9和280Tg,1991年大气甲烷的体积分数和年排放总量分别为1611.9×10-9和533.9Tg。而对流层中OH的数密度则由1840年的7.17×105cm-3变化到1991年的5.79×105cm-3,下降了19%。如果CH4、CO及NOx这三种排放源继续按给定的方案增长,那么到2020年大气甲烷的体积分数和年排放总量将增加为2090.7×10-9和966.2Tg,而OH的数密度将为5.47×105cm-3,比1840年降低24%。 相似文献
2.
大气中一氧化碳浓度变化的模拟研究 总被引：4，自引：1，他引：4
应用全球二维大气化学模式,模拟了CO、CH4和OH自由基等成分自工业革命到2020年的长期变化.模拟的全球CO平均体积分数在1840年、1991年和2020年分别为27×10-6、76×10-6和105×10-6.从1840到1991年,OH自由基数浓度从7.17×105个分子/cm3下降到5.79×105个分子/cm3,降低了19%.模拟的CH4长期变化与冰芯资料相符.模拟的20世纪80年代CO体积分数年增长率为1.03%～1.06%.大气中CO在20世纪90年代前是增长的,而到90年代初观测到CO体积分数突然下降.应用二维大气化学模式对此原因进行了模拟研究,结果表明,CO排放源的减少是CO体积分数下降的主要因子,平流层臭氧减少是另一个重要因子.尽管CO排放源的减少对大气CH4增长率的变化有较大影响,而CH4排放源减少对CO体积分数变化却几乎没有影响. 相似文献
3.
用气相色谱法在瓦里关全球基准站进行了大气甲烷（CH4）的连续测量,结合NOAA/CMDL气瓶采样CH4浓度资料的分析结果,给出了我国内陆高原大气CH4本底浓度的变化特征。分析结果表明:瓦里关山大气CH4浓度在1780×10-9～1840×10-9范围内波动,浓度值的变化范围符合中高纬度地区CH4浓度分布;CH4浓度有明显的日变化,夏季的变化趋势及振幅与冬春季有所不同;季节变化幅度不大,与全球大气CH4浓度本底值季节变化的特征及变化幅度的地理分布不太一致;有明显的年际变化,CH4年平均浓度表现为逐年升高,年 相似文献
4.
北京大气甲烷季变化及发展趋势 总被引：9，自引：1，他引：8
近年来北京大气中CH4含量仍在上升,但平均增长率已从1985～1989年的1.76%.a-1,下降到1990～1997年的0.50%.a-1;冬季和夏季两次出现峰值,表现出明显的双峰模态季节变化。但北京大气CH4变化的最大特点是年际季变化不均一,12年中,北京大气CH4共计增长185×10-9混和体积比,其中冬季增长的贡献为69×10-9混和体积比,约占总增长的37%;而夏季的增长贡献不足40×10-9混和体积比,约占总增长的21%。90年代以后,北京大气CH4增长率进一步减慢,主要原因是生物源排放不再增加,而非生物源排放量的增长是大气CH4继续增长的主要原因。 相似文献
5.
1992年大气甲烷增长速率异常
下降的模拟研究 总被引：4，自引：0，他引：4
应用初步建立的全球二维大气化学模式,模拟了甲烷、一氧化碳和OH自由基自工业革命以来的长期变化,对1992年大气中甲烷增长速率突然下降这一异常现象的可能原因如平流层O3下降,皮纳图博火山引起对流层温度下降、甲烷排放源减少等逐一进行了定量研究。研究还发现一氧化碳排放源的减少是另一重要影响因子,并进行了验证。结果表明,1992年甲烷增长速率急剧下降的主要原因来自甲烷和一氧化碳排放源的减少。 相似文献
6.
O3,CO2浓度及太阳光谱变化对作物光合作用影响的数值模拟研究 总被引：4，自引：2，他引：4
对光合作用 蒸腾作用 气孔调节进行耦合 ,从生物化学尺度扩展至冠层尺度 ,发展了一个冬小麦冠层光合作用生态动力模式 ,模式考虑了O3,CO2 和光谱变化对作物光合的综合影响。利用美国光合作用实测资料对模式进行验证 ,叶片模式通过了相关显著性检验并具有较高的准确度。数值分析表明 :当O3 浓度由 0× 10 -9V/V上升至2 0 0× 10 -9V/V时 ,冠层光合速率下降 2 9%左右 ;当CO2 浓度由 330× 10 -6V/V上升至 6 6 0× 10 -6V/V时 ,冠层光合速率增加大约 37% ;当光谱比例系数由目前的 0 .5下降至 0 .4时 ,冠层光合速率将下降 2 7%左右。对于污染严重、易发生光化学烟雾的城郊附近 ,在阳光强烈的典型晴天 ,中午O3 浓度达到 2 0 0× 10 -9V/V时 ,即使气候条件不发生改变 ,CO2 浓度对作物光合作用的正效应也不足以弥补O3 浓度升高所造成的负效应 ,冠层光合速率将比目前干洁地区略有下降 ,如果进一步考虑光合作用有效辐射光谱成分下降至 0 .4左右 ,冠层光合作用将比目前的BASE值下降 35 %左右。 相似文献
7.
CH4是仅次于CO2的重要温室气体。2006年9月至2008年8月期间,按全球大气本底观测要求,在青海瓦里关、北京上甸子、浙江临安和黑龙江龙凤山4个国家级野外站开展每周一次空气样品flask瓶采样分析,获得了该地区为期2 a的大气CH4本底浓度资料。结果表明,2 a间瓦里关、上甸子、临安和龙凤山4站CH4浓度年均增幅分别为9.1×10-9、3.8×10-9、21.8×10-9和8.2×10-9;瓦里关站大气CH4浓度增长趋势与全球平均状况较为接近,能较好地反映北半球中高纬度内陆地区大气本底特征;但上甸子站年均本底值相对较低且季振幅偏小,而龙凤山和临安站季节变化规律相似,表现为CH4浓度冬季高而夏季偏低且季振幅较大。 相似文献
8.
OH自由基是对流层中主要的氧化剂，是大气氧化性的重要表征。文章利用GEOS-Chem模式量化了2014～2017年“大气污染防治行动计划”执行以来，人为排放和气象因素变化对中国夏季大气OH浓度变化的贡献。模拟结果表明，2014～2017年间夏季整个中国OH浓度呈现上升趋势，最大上升出现在30°N附近的华南地区。在华北平原地区，OH浓度也呈明显的上升趋势(0.1×106 molecules cm-3 a-1)，而OH浓度比较高的珠江三角洲地区的OH变化趋势较小。敏感性试验结果表明，气象和人为排放变化都对2014～2017年华北平原OH浓度上升有促进作用，但人为排放的贡献(OH增加10.0%)远大于气象的贡献(OH增加1.5%);OH浓度变化最大的南方地区主要是气象条件控制。进一步对气象因素分析发现，影响全国OH变化最重要的气象要素是太阳短波辐射，决定了2014～2017年中国OH浓度增长趋势最大的区域。但在华北地区，2014～2017年短波辐射略微减少的影响被边界层高度明显降低带来的OH增加所抵消。 相似文献
9.
1 设备和方法试验设计 5个Ｏ3浓度 ,分别为处理Ａ :2 0 0× 1 0 - 9、处理Ｂ :1 0 0× 1 0 - 9、处理Ｃ :50× 1 0 - 9、处理Ｄ :背景大气中的Ｏ3浓度 ( 2 5× 1 0 - 9～ 48× 1 0 - 9,并随天气情况和昼夜变化 )、处理Ｅ :经活性炭过滤后的纯净空气 (Ｏ3浓度低于 1 0× 1 0 - 9)。冬小麦种子 (京冬 6号 )于 1 998年 1 0月 3日在直径 36ｃｍ ,高度 2 6ｃｍ的瓦盆中播种。盆内土壤质地均匀且一致 ,全生育期管理方法相同 ,水肥条件适宜 ,无病虫害和杂草危害。1 999年 4月 3日 (起身—拔节 )开始进行不同Ｏ3浓度的熏气处理 ,熏气时间为每天 9:0… 相似文献
10.
瓦里关温室气体本底研究的主要进展 总被引：11，自引：0，他引：11
由于温室气体浓度显著增长及其在气候与环境变化中的作用,国际上众多的科学计划和观测体系都把它们的时空分布、源汇及趋势列为重要内容,获得的各种资料在评价人类活动对气候和环境的影响及有关对策研究中起着关键作用。文章阐述了在中国内陆本底地区开展温室气体长期、定点观测的意义和必要性,系统地讨论了10多年来中国瓦里关本底站温室气体本底研究的主要进展。利用瓦里关经严格国际比对和质量控制的大气CO2、CH4长期观测资料,结合同期的地面风资料进行统计分析,建立了瓦里关大气CO2和CH4本底资料筛选方法;利用本底观测资料,研究了瓦里关大气CO2及其δ13C、CH4和CO本底变化及源汇特征所体现的亚洲内陆地域特点和全球代表性,并进一步与同期、同纬度海洋边界层参比值(MBL)以及北半球其他6个大气本底站同期观测数据对比分析,发现了瓦里关大气CH4和CO独特的季节变化并探讨了成因;根据空气团后向轨迹簇所途经的下垫面源汇同观测的大气CO2和CH4浓度变化之间的关系,探讨了瓦里关大气CO2和CH4的输送来源;利用Hysplit-4扩散与输送模式,计算了冬、夏典型月份人为源和自然生态系统源汇对瓦里关大气CO2浓度变化的贡献。并在现有基础上,提出了有待进一步解决的科学问题。 相似文献
11.
A global two-dimensional chemistry model is developed to study long-term trends of CH4 since industrial revolution.The sources of CH4,CO and NOx are parameterized as functions of latitude and time.With two long-term emission scenarios,long-term trends of CH4 are simulated.The results have a good agreement with observation from ice cores.The modeled CH4 increased from 760 ppbv in 1840 to 1611.9 ppbv in 1991, while the modeled number concentration of tropospheric OH decreased from 7.17×105 cm-3 in 1840 to 5.79×105 cm-3 in 1991.The increase of atmospheric CH4 can be explained by the increase of emission of CH4 and build-up because of decrease of OH radicals that remove CH4 from the atmosphere.The model is also used to simulate the distribution of CH4.Comparisons between the model results and observations show that the model can simulate both latitudinal distribution and seasonal variation of CH4 well. 相似文献
12.
Alexandre Kukui Gérard Ancellet Georges Le Bras 《Journal of Atmospheric Chemistry》2008,61(2):133-154
A new version of an atmospheric pressure chemical ionisation mass spectrometer has been developed for ground based in situ
atmospheric measurements of OH and total peroxy (HO2 + organic peroxy) radicals. Based on the previously developed principle of chemical conversion of OH radicals to H2SO4 in reaction with SO2 and detection of H2SO4 using an ion molecule reaction with NO3─, the new instrument is equipped with a turbulent chemical conversion reactor allowing for measurements in moderately polluted
atmosphere at NO concentrations up to several ppb. Unlike other similar devices, where the primary NO3─ ions are produced using radioactive ion sources, the new instrument is equipped with a specially developed corona discharge
ion source. According to laboratory measurements, the overall accuracy and detection limits are estimated to be, respectively,
25% and 2 × 105 molecule cm-3 for OH and 30% and 1 × 105 molecule cm-3 for HO2 at 10 min integration times. The detection limit for measurements of OH radicals under polluted conditions is 5 × 105 molecules cm-3 at 10 min integration times. Examples of ambient air measurements during a field campaign near Paris in July 2007 are presented
demonstrating the capability of the new instrument, although with reduced performance due to the employment of non isotopic
SO2. 相似文献
13.
目前温室气体清单的编制主要基于IPCC方法,该方法用于特定城市或区域清单编制时可能会引起较大的不确定性,而目前对城市/区域尺度清单的不确定性的分析还存在很大的欠缺。本文通过南京市和长三角温室气体排放因子甄选,应用IPCC方法计算了2009年南京市和长三角的人为温室气体排放量,并以其为个例利用蒙特卡洛方法开展城市和区域尺度的温室气体人为排放清单不确定性的初步探究。研究结果表明:南京市CH4和CO2排放量的95%的概率分布范围分别为(1.08~1.86)×105t和(6.50~7.41)×107t,不确定性分别为-21.74%~34.78%和-7.01%~5.87%;长三角CH4和CO2排放量的95%的概率分布范围分别为(4.07~5.89)×106t和(1.62~1.82)×109t,不确定性分别为-15.60%~22.24%和-6.04%~5.34%。 相似文献
14.
Eric Schlosser Birger Bohn Theo Brauers Hans-Peter Dorn Hendrik Fuchs Rolf Häseler Andreas Hofzumahaus Frank Holland Franz Rohrer Lutz Olaf Rupp Manfred Siese Ralf Tillmann Andreas Wahner 《Journal of Atmospheric Chemistry》2007,56(2):187-205
At the atmosphere simulation chamber SAPHIR in Jülich both Laser-Induced Fluorescence Spectroscopy (LIF) and Long-Path Differential
Optical Laser Absorption Spectroscopy (DOAS) are operational for the detection of OH radicals at tropospheric levels. The
two different spectroscopic techniques were compared within the controlled environment of SAPHIR based on all simultaneous
measurements acquired in 2003 (13 days). Hydroxyl radicals were scavenged by added CO during four of these days in order to
experimentally check the calculated precisions at the detection limit. LIF measurements have a higher precision (σ= 0.88×106 cm–3) and better time resolution (Δt = 60 s), but the DOAS method (σ= 1.24×106 cm–3, Δt = 135 s) is regarded as primary standard for comparisons because of its good accuracy. A high correlation coefficient of
r = 0.95 was found for the whole data set highlighting the advantage of using a simulation chamber. The data set consists of
two groups. The first one includes 3 days, where the LIF measurements yield (1 – 2) ×106 cm–3 higher OH concentrations than observed by the DOAS instrument. The experimental conditions during these days are characterized
by increased NOx concentration and a small dynamic range in OH. Excellent agreement is found within the other group of 6 days. The regression
to the combined data of this large group yields unity slope without a significant offset. 相似文献
15.
G. Solignac I. Magneron A. Mellouki A. Muñoz M. Martin Reviejo K. Wirtz 《Journal of Atmospheric Chemistry》2006,54(2):89-102
A study of the oxidation mechanism of N-methyl pyrrolidinone (C5H9NO, NMP) initiated by hydroxyl radicals was made at EUPHORE at atmospheric pressure (1000 ± 10) mbar of air and ambient temperature (T = 300 ± 5 K). The main products were N-methyl succinimide (NMS) (52 ± 4)% and N-formyl pyrrolidinone (FP) (23 ± 9)%. The relative rate technique was used to determine the rate constants of OH with NMP, NMS and FP, the measured values were (in units of cm3 molecule
− 1 s− 1): kNMP = (2.2 ± 0.4) × 10− 11, kNMS = (1.4 ± 0.3) × 10− 12 and kFP = (6 ± 1) × 10− 12. The results are presented and discussed in terms of the atmospheric impact. 相似文献
16.
The 1,4-hydroxycarbonyl 5-hydroxy-2-pentanone is an important product of the gas-phase reaction of OH radicals with n-pentane in the presence of NO. We have used a relative rate method with 4-methyl-2-pentanone as the reference compound to measure the rate constant for the reaction of OH radicals with 5-hydroxy-2-pentanone at 296 ± 2 K. The carbonyls were sampled by on-fiber derivatization using a Solid Phase Micro Extraction (SPME) fiber coated with O>
-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine hydrochloride with subsequent thermal desorption of the oxime derivatives and quantification by gas chromatography with flame ionization detection. For comparison, the reference compound was also analyzed following sample collection onto a Tenax adsorbent cartridge. Products of the reaction were investigated using coated-fiber SPME sampling with gas chromatography-mass spectrometry analysis as well as by using in situ atmospheric pressure ionization mass spectrometry. A rate constant for the reaction of OH radicals with 5-hydroxy-2-pentanone of (1.6 ± 0.4) × 10–11 cm3 molecule–1 s–1 was obtained at 296 ± 2 K. Two dicarbonyl products, of molecular weight 86 and 100, were observed and are attributed to CH3C(O)CH2CHO and CH3C(O)CH2CH2CHO, respectively. Reaction schemes leading to these products are presented. 相似文献
17.
K.-Y. Wang J. A. Pyle D. E. Shallcross D. J. Larry 《Journal of Atmospheric Chemistry》2001,38(1):31-71
In part two of this series of papers on the IMS model, we present the chemistry reaction mechanism usedand compare modelled CH4, CO, and O3 witha dataset of annual surface measurements. The modelled monthly and 24-hour mean tropospheric OH concentrationsrange between 5–22 × 105 moleculescm–3, indicating an annualaveraged OH concentration of about 10 × 105 moleculescm–3. This valueis close to the estimated 9.7 ± 0.6 × 105 moleculescm–3 calculated fromthe reaction of CH3CCl3 with OH radicals.Comparison with CH4 generally shows good agreementbetween model and measurements, except for the site at Barrow where modelledwetland emission in the summer could be a factor 3 too high.For CO, the pronounced seasonality shown in the measurements is generally reproduced by the model; however, the modelled concentrations are lower thanthe measurements. This discrepancy may due to lower the CO emission,especially from biomass burning,used in the model compared with other studies.For O3, good agreement between the model and measurements is seenat locations which are away from industrial regions. The maximum discrepancies between modelled results and measurementsat tropical and remote marine sites is about 5–10 ppbv,while the discrepancies canexceed 30 ppbv in the industrial regions.Comparisons in rural areas at European and American continental sites arehighly influenced by the local photochemicalproduction, which is difficult to model with a coarse global CTM.The very large variations of O3 at these locations vary from about15–25 ppbv in Januaryto 55–65 ppbv in July–August. The observed annual O3amplitude isabout 40 ppbv compared with about 20 ppbv in the model. An overall comparison of modelled O3 with measurements shows thatthe O3seasonal surface cycle is generally governed bythe relative importance of two key mechanisms that drivea springtime ozone maximum and asummertime ozone maximum. 相似文献
18.
Rate constants for the gas-phase reactions of OH radicals, NO3 radicals and O3 with the C7-carbonyl compounds 4-methylenehex-5-enal [CH2=CHC(=CH2)CH2CH2CHO], (3Z)- and (3E)-4-methylhexa-3,5-dienal [CH2=CHC(CH3)=CHCH2CHO] and 4-methylcyclohex-3-en-1-one, which are products of the atmospheric degradations of myrcene, Z- and E-ocimene and terpinolene, respectively, have been measured at 296 ± 2 K and atmospheric pressure of air using relative rate methods. The rate constants obtained (in cm3 molecule–1 s–1 units) were: for 4-methylenehex-5-enal, (1.55 ± 0.15) × 10–10, (4.75 ± 0.35) × 10–13 and (1.46 ± 0.12) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3Z)-4-methylhexa-3,5-dienal: (1.61 ± 0.35) × 10–10, (2.17 ± 0.30) × 10–12, and (4.13 ± 0.81) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3E)-4-methylhexa-3,5-dienal: (2.52 ± 0.65) × 10–10, (1.75 ± 0.27) × 10–12, and (5.36 ± 0.28) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; and for 4-methylcyclohex-3-en-1-one: (1.10 ± 0.19) × 10–10, (1.81 ± 0.35) × 10–12, and (6.98 ± 0.40) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively. These carbonyl compounds are all reactive in the troposphere, with daytime reaction with the OH radical and nighttime reaction with the NO3 radical being predicted to dominate as loss processes and with estimated lifetimes of about an hour or less. 相似文献
19.
Barnes I. Bastian V. Becker K. H. Fink E. H. Nelsen W. 《Journal of Atmospheric Chemistry》1986,4(4):445-466
The reactions of OH radicals with SO2, H2S, thiophenol, and a series of aliphatic thiols (1–5 C-atoms) have been investigated in 201 and 381 reaction chambers at 1 atm total pressure and 300 K using a competitive kinetic technique. Initially, OH radicals were produced by photolysis of CH3ONO/NO mixtures in air. Applying this OH source rate constants for OH with SO2, H2S, and thiophenol in synthetic air were determined to be (1.1±0.2)×10-12, (5.5±0.8)×10-12 and (1.1±0.2)×10-11 cm3 s-1, respectively. However, when this method was applied to the aliphatic thiols the rate constants obtained were found to be dependent on the partial pressures of O2 and NO. These effects have been attributed to the built-up of a radical species, not yet identified, which leads to uncontrolled chain reactions in the system. Using the photolysis of H2O2 at wavelengths greater than 260 nm as the OH source in 1 atm N2, rate constants for the 1–5 aliphatic thiols in the range 2.9 to 5.6×10-11 cm3 s-1 were obtained. The rate constants obtained in the present study are compared with recent literature values. 相似文献
20.
D. Perner U. Platt M. Trainer G. Hübler J. Drummond W. Junkermann J. Rudolph B. Schubert A. Volz D. H. Ehhalt K. J. Rumpel G. Helas 《Journal of Atmospheric Chemistry》1987,5(2):185-216
Using long path UV absorption spectroscopy we have measured OH concentrations close to the earth's surface. The OH values observed at two locations in Germany during 1980 through 1983 range from 0.7×106 to 3.2×106 cm-3. Simultaneously we measured the concentrations of O3, H2O, NO, NO2, CH4, CO, and the light non methane hydrocarbons. We also determined the photolysis rates of O3 and NO2. This allows calculations of OH using a zero dimensional time depdendent model. The modelled OH concentrations significantly exceed the measured values for low NO
x
concentrations. It is argued that additional, so far unidentified. HO
x
loss reactions must be responsible for that discrepancy. 相似文献