中国区域大气本底站近地面臭氧来源贡献及区域代表性

回顾了关于长距离输送对中国区域本底大气臭氧的影响,以及中国区域大气本底站臭氧变化及其区域代表性两方面的研究进展。来自不同污染源区O₃的长距离输送对中国区域O₃影响的研究结果分歧较大,贡献最显著的源区和受体地区也存在争议;同时,鲜有研究考虑到平流层对对流层的O₃贡献,而这部分贡献在前体物排放很少的本底地区非常重要。中国区域各大气本底观测站分别与其周围一定范围内的区域具有相同的对流层O₃柱浓度最大值月份分布,而对与人体健康密切相关的近地面O₃区域特征的分析尚未深入开展;鉴于研究方法的局限性,也尚未深入揭示形成O₃变化区域特征的复杂成因。基于现有研究进展和不足之处,如何利用全球大气化学-环流模式的示踪模拟结果,定量评估来自全球不同地区的O₃对中国本底大气O₃的影响,并进一步评估中国区域6个大气本底站近地面O₃季节变化的区域代表性,是亟待解决的科学问题。     

The Effect of Temperature and Humidity on the Reaction of Ozone with Combustion Soot: Implications for Reactivity near the Tropopause

The effect of temperature (296–238 K) on the reaction of combustion soot (n-hexane) with ozone at low concentration (6–8 ppm) has been measured. Long optical path FTIR spectroscopy has revealed the rate law for ozone loss beyond initial stages, second order in O₃, to be the same over this range of conditions. The reaction rate is 3.5 times lower at 238 K than at 296 K, and reveals an activation energy of 12.9 ± 0.5 kJ mol^–1. The effect of humidity on the reaction has been estimated using its recently determined rate law dependence (p^0.2). These data, differing from O₃ reaction kinetics obtained from other types of carbonaceous particles used as surrogates for atmospheric soot, have implications for the role of combustion soot in atmospheric chemistry. Any involvement of aircraft soot in ozone depletion near the tropopause, for example, should be estimated using these temperature and humidity dependences.     

Summertime Surface N2O Concentration Observed on FildesPeninsula Antarctica： Correlation with TotalAtmospheric O3 and Solar Activity

Three-year summertime surface atmospheric N2O concentrations were observed for the first timeon the Fildes Peninsula, maritime Antarctica, and the relationships among the N2O concentration, totalatmospheric O3 amount, and sunspot number were analyzed. Solar activity had an important effecton surface N20 concentration and total O3 amount, and increases of sunspot number were followed bydecreases in the N2O concentration and total O3 amount. A corresponding relationship exists betweenthe N2O concentration and total atmospheric O3, and ozone destruction was preceded by N2O reduction.We propose that the extended solar activity in the Antarctic summer reduces the stratospheric N2O byconverting it into NOx, increases the diffusion of N2O from the troposphere to the stratosphere, decreasesthe surface atmospheric N2O, and depletes O3 via the chemical reaction between O3 and NOx. Ourobservation results are consistent with the theory of solar activity regarding the formation of the AntarcticO3 hole.     

MEASUREMENTS AND MODEL SIMULATIONS OF SURFACE OZONE VARIATIONS AT DIFFERENT BACKGROUND CONCENTRATIONS OF THE PRECURSORS*

Ozone photochemical production and loss in very different environments at Waliguan baseline station and Lin'an background station were simulated by using the measurement data and photochemical box model.The results show that net ozone photochemical production rate is negative,about 0.5 ppb/d,at Waliguan baseline sation,because of very low precursor concentrations.But at Lin'an background station,the net photochemical ozone production is positive,about 2-3 ppb/h.which is very closed with the measurement at Lin'an.That means ozone production was controlled by photochemical reactions at Lin'an background station,because of the higher precursor concentrations.The net destruction rate,at Waliguan Mt.,is not large,so that future increase in anthropogenic emission of reactive nitrogen will lead to larger production rates of steady-state O₃ concentration.     

2020年新冠肺炎疫情管控期江苏省大气污染物浓度变化特征

利用江苏省大气环境监测站点的大气污染物监测数据,分析了2020年初新冠肺炎疫情管控期间(2—3月)主要大气污染物浓度的变化特征。结果显示,相比于2019、2020年疫情管控期间PM_2.5、PM₁₀、NO₂、SO₂、CO浓度的全省平均降幅分别为37.5%、36.9%、31.9%、28.2%和21.2%。严格管控期的2月和生产恢复期的3月,江苏省十三市PM_2.5、PM₁₀浓度同比降幅大致相当,呈现出较好的时间连续性和空间均匀性。但各市臭氧浓度同比变化呈现出较大的时空差异。空间上,沿江以南城市南京、无锡、常州、苏州和镇江五市臭氧浓度明显上升,而其他城市臭氧浓度以下降为主;时间上,2月南京等九市臭氧浓度上升,3月徐州等八市臭氧浓度持平或者下降。假设未发生新冠肺炎疫情以及未采取为阻断疫情蔓延而实施的种种举措,在仅考虑近年来大气污染防治政策持续实施的情况下,与预期降幅相比,疫情管控对NO₂实况浓度降幅的影响最大,其次是PM_2.5     

北京市夏季臭氧变化特征的观测研究

利用2002年7月至8月325m气象塔资料研究了北京市夏季近地层臭氧浓度变化特征及其与气象因子的关系。结果表明：北京市夏季边界层臭氧浓度日变化显著．臭氧浓度随高度增加而增加；臭氧多数为单峰型分布，双峰型仅分布在底层；臭氧峰值出现时间与气温峰值出现时间基本一致，或略有落后。     

NO_x的准两年周期变化及其与臭氧准两年周期振荡的关系 II.模拟研究

利用NCAR的包含化学、辐射、动力相互作用的二维模式就纬向风的准两年周期振荡 (简称QBO)对平流层微量元素分布的影响进行数值模拟试验。模拟中 ,输入纬向风QBO的值 ,计算出NOx、臭氧浓度和各种气象要素的垂直经向分布 ,并与不考虑QBO强迫的数值模拟结果进行对比。在第I部分HALOE资料分析的基础上 ,进一步讨论了在纬向风QBO的影响下NOx浓度垂直分布的变化及其准两年周期振荡 ,并研究了NOx的QBO与臭氧QBO的关系。结果表明 :模拟六年平均的NOx混合比分布与观测结果基本一致 ,并且在纬向风场QBO强迫下 ,NOx混合比扰动有明显的准两年周期振荡 ;与臭氧的QBO比较 ,发现在2 8km以下 ,NOx的QBO与臭氧QBO同位相 ,而在 2 8km以上 ,它们则是反位相 ,与HALOE资料的观测结果基本吻合。文中对模拟得到的由于风场QBO引起的余差环流输送作用做了进一步的分析 ,并讨论了在不同高度的气层中余差环流的输送作用与NOx破坏作用在臭氧QBO形成中的相对重要性     

Harmonious Inter-decadal Changes of July–August Upper Tropospheric Temperature Across the North Atlantic, Eurasian Continent,and North Pacific

The authors have developed an integral view of the inter-decadal variability of July–August(JA)tro- pospheric temperature across the entire subtropical Northern Hemisphere.Using reanalysis data and com- plementary balloon-borne measurements,the authors identify one major mode of variability for the period 1958–2001 which exhibits a significant cooling center over East Asia and warming centers over the North Atlantic and North Pacific.The cooling(warming)signals barotropically penetrate through the troposphe...     

Spatial patterns of Tropospheric Biennial Oscillation and its numerical simulation

In order to investigate the spatial patterns of the Tropospheric Biennial Oscillation （TBO） on the global scale, the Climate Prediction Center （CPC） Merged Analysis of Precipitation （CMAP） monthly averaged precipitation and the Climate Diagnostics Center （CDC） monthly outgoing long-wave radiation （OLR） and SST are used in conjunction with TBO bandpass-filtering. The results indicate active biennial variability in the tropical eastern-central Pacific regions. It is evident that observations reflect the biennial component of the ENSO rather than the TBO itself. Since some studies have pointed out that the TBO is a broad-scale phenomenon differing from the ENSO, to investigate the pure TBO the ENSO signal must be excluded. The Scale Interaction Experiment-FRCGC （SINTEX-F） coupled general circulation model （CGCM） developed at Japan Frontier Research Center for Global Change （FRCGC） can capture both the ENSO and the biennial signals. Air-sea interactions in the tropical eastern-central Pacific are decoupled to eliminate the effects of ENSO in a experiment by SINTEX-F and the results show that biennial variability still exists even without ENSO. It seems to mean that the TBO and ENSO are independent from each other. Furthermore, the model results indicate that the two key regions are southwest Sumatra and the tropical western Pacific for the TBO cycle.