Simulated seasonal variations in nitrogen wet deposition over East Asia

近20年来我国的酸雨和酸沉降分布发生了较大变化,其中一个重要变化是硝酸根离子明显增加,这主要是氮氧化物排放增加所导致的。为了评估氮氧化物排放对酸雨和酸沉降的影响,本文利用区域大气化学模式RAMS-CMAQ模拟分析了东亚地区氮氧化物排放、输送和化学转化过程以及降水时空变化对氮氧化物和氮沉降量时空分布的影响,并借助于中国气象台站和东亚酸沉降监测网的观测数据评估了模式结果的合理性。模拟结果显示,东亚地区氮湿沉降的季节变化十分显著,氮湿沉降通量在1~18 kg N ha~(-1) yr~(-1)之间;春夏两季湿沉降占全年的71%,其中夏季占42.7%。     

华北地区大气氮沉降的空间格局和季节特征（英文）

作为农业集约化和经济快速发展的地区之一,华北地区较高的氮沉降不容忽视。本文利用卫星观测的对流层柱浓度和大气化学传输模型模拟的剖面信息,研究了华北地区氮沉降的空间格局和季节特征。结果表明,华北地区总氮沉降通量为16.3–106.5 kg N ha~(-1)yr~(-1),平均为54.5±17.2 kg N ha~(-1)yr~(-1)。高值区主要集中在城市和农田,低值区主要集中在人类活动较少的森林和草地。在总氮沉降量中,湿沉降量占36%;颗粒物干沉降量占12%;气态干沉降占52%。对于干沉降来说,气态HNO_3和颗粒物NO_3~-在冬季和秋季较高,春季和夏季较低。与之相反,气态NH_3和颗粒物NH_4~+在春季和夏季较高,冬季和秋季较低。这可能是NO_x和NH_3排放源和排放强度的季节差异造成的。另外,气态NO2沉降没有明显的季节变化。湿沉降主要受降水影响,呈现夏季高,冬季低的季节变化。本研究为华北地区总氮沉降提供了客观的空间格局和季节特征的见解。     

大城市气溶胶对光化辐射通量及臭氧的影响研究(Ⅱ)——数值试验分析

城市化已引起大量痕量气态污染物、气溶胶以及臭氧前体物的人为排放,从而引起区域大气化学循环的扰动变化。在分析国内外研究现状与观测实例的基础上,进一步用辐射模式与化学模式研究了气溶胶对到达地面的光化辐射通量以及臭氧形成的影响,表明气溶胶可显著减小到达地面的光化学辐射通量,减缓光化学反应进程,并进一步抑制臭氧的形成;在目前广州等大城市的污染过程中,高浓度的气溶胶可造成光化学辐射通量衰减高达70%~80%,紫外线的衰减比可见光更明显,在可见光波段随波长增大衰减幅度减小,气溶胶层的存在对短波长激发的光化学过程的影响更加显著。分析说明城市污染大气中光化学反应的生成物与反应物之间存在自抑制过程,在目前的城市群复合污染情况下,气溶胶与臭氧之间的非线性相互作用值得关注。     

中国西南和华南地区硫沉降数值模拟

利用CMAQ(Community Multi-scale Air Quality)模式模拟了中国西南和华南地区的硫沉降。模式中详细考虑了气象过程、气相与液相化学过程、非均相化学过程、气溶胶过程和干湿沉降过程对SO2输送、转化和沉降过程的影响。通过与IMPACTS小流域的观测资料的比较,显示了该模式系统能够较好地模拟SO2在大气中的转化以及干湿沉降过程。在此基础之上,分析了不同季节该区域的硫沉降和向外输送的情况,并且模拟了该区域2002年全年的硫沉降分布状况,这为该区域有效地污染治理奠定了基础。     

积云对流和云物理过程调整对气候模拟的影响

本文利用中国科学院大气物理研究所大气科学和地球流体力学数值模拟国家重点实验室 (LASG/IAP) 的大气环流谱模式SAMIL, 结合观测与政府间气候变化专门委员会第四次评估报告 (IPCC AR4) 大气模式集合平均结果, 以大气辐射通量为例, 诊断分析了物理过程调整前后模式对气候模拟的影响。旧版本SAMIL对大气辐射通量的模拟存在较大偏差, 经过大气辐射过程、 积云对流和诊断云等物理过程的调整后, 新版本SAMIL模拟的全球辐射通量的年平均结果与观测的偏差大幅减小, 其中大气顶能量收支的年变化及其平均值与观测更为接近。在积云对流方案调整基础上, 通过对诊断云物理方案的进一步调整, 新版本SAMIL对云物理量模拟更为合理, 在赤道辐合带等区域, 在很大程度上克服了单一积云对流物理过程调整引起的云宏观和微观属性不匹配问题, 能模拟出夏季气候平均辐射通量的全球分布特征, 尤其在东亚区域有较好的模拟能力。研究还表明, 在热带和副热带对流活跃区域, 当前SAMIL中积云对流过程偏差对辐射通量的模拟偏差有很大影响, 而模式中较为简单的诊断云方案也会将云宏观物理量模拟偏差带入云微观量模拟中, 也是主要偏差源之一。本文结果表明, 要继续提高SAMIL的模拟性能, 急需更新云物理参数化方案以改进云辐射过程的模拟, 同时也需要有针对性的研究积云对流和云物理过程之间相互作用, 并作进一步协同调整。     

农田生态系统大气硫沉降通量的观测研究

1998年 11月～ 1999年 10月间在中国科学院红壤站 (江西鹰潭 )农田小气候站进行了大气二氧化硫 (SO2 )、硫酸盐粒子 (SO2 -4)浓度采样和雨水样本收集 ,利用阻力模式和全年逐时气象资料计算 SO2 和 SO2 -4的干沉降速度 ,估算干沉降通量 ,利用降水资料和雨水中硫酸根离子浓度估计大气硫的湿沉降 ,从而定量研究大气硫沉降输入农田生态系统的通量 ,结果表明 :农田下垫面上 SO2 和 SO2 -4干沉降速度的年平均值分别是 0 .373± 0 .170 cm· s-1(月均值 0 .16 1～ 0 .5 45 cm·s-1)、0 .198± 0 .12 3cm· s-1(月均值 0 .15 2～ 0 .2 6 9cm· s-1)。农田下垫面硫年总沉降量为 10 .3g· m-2 ,其中干沉降占总沉降的 83.3%。硫的干沉降又以 SO2 的干沉降为主 ,占年干沉降总量的 92 .2 %。大气硫沉降输入占农田生态系统输入总量的 90 %以上 ,是农田生态系统获取硫素的一个重要途径     

Wet deposition and scavenging ratio of air pollutants during an extreme rainstorm in the North China Plain

大气湿沉降是陆地和水体环境中营养成分和有毒物质的重要来源。以往湿沉降研究较多关注年尺度或年际变化,极端降水事件鲜见报道。通过实验观测,发现2016年7月19–21日华北极端暴雨(北京观测站325.6 mm)有效清除了区域大气颗粒物,但不同化学成分被湿清除的效率存在差异(无机离子比有机物和气态污染物更容易被湿清除)。此次极端降水铵盐和硝酸盐的湿沉降通量占北京全年的22%和4%,相当于青藏高原一年的氮沉降。考虑到气候背景下极端暴雨出现的频次,极端降水的生态环境影响需要更精细化的评估。     

南海海域海-气耦合模式及其数值模拟试验

在ＮＣＡＲ区域气候模式ＲｅｇＧＭ２和普林斯顿海洋模式ＰＯＭ基础上发展适用于区域海－气相互作用研究的区域海－气耦合模式,模式采用同步耦合、海洋模式将海表温度提供给大气模式,大气模式为海洋模式提供太阳短波辐射、感热能量、潜热通量。海洋与大气模式每１５ｍｉｎ交换一次通量。耦合过程没有使用通量校正。使用该模式对中国南海区域１９９５年５－７月大气和海洋进行了模拟试验,将模拟结果与ＣＯＡＤＳ通量强迫的模拟结果     

用STEM—Ⅱ模式研究东亚地区春季沙尘气溶胶对硫化物输送和沉降的影响

利用ＳＴＥＭ－ＩＩ三维区域尺度大气化学模式,研究了１９９４年３月１日至１４日东亚地区春季沙尘气溶胶对硫化物输送和沉降的影响。结果表明,ＳＯ２和ＳＯ２４的大值区主要出现在我国东部地区。在模拟时段,日本地区火山源的排放对该地区大气中Ｓ分布的贡献达１０％～３０％。并与当时飞机的观测结果相吻合。模拟区域内ＳＯ２和ＳＯ２４的收支的分析研究表明,在硫的总排放量中,从东边界面流出去的输送通量最大,并出现在３０～４００Ｎ带的２～６ｋｍ高度上,这是与该地区最大的人为排放源所在地相一致的。最后,给出了模拟时段整个对流层大气ＳＯ２－４气溶胶含量的分布,还仨算了ＳＯ２－４气溶胶对地气系统的直接辐射强迫和温度变化的影响。     

长江三角洲地区净生态系统二氧化碳通量及浓度的数值模拟

净生态系统碳通量(NEE)的计算对于准确模拟区域碳通量和大气CO₂浓度的时空变化至关重要。本文利用中尺度大气-温室气体耦合模式WRF-GHG(Weather Research and Forecasting Model with Greenhouse Gases Module),对2010年7月28日至2010年8月2日期间影响长江三角洲地区大气CO₂浓度及时空分布的各种过程进行了详尽模拟。结果表明,植被光合呼吸模型(VPRM)能模拟不同植被下垫面NEE的日变化;WRF-GHG模拟的大气CO₂浓度日变化与观测相吻合,但低估了大气CO₂浓度5~15 ppm(ppm表示10-6),这可能与人为排放源的低估、VPRM参数的不确定性以及气象场模拟的不准确性有关。太湖和植被覆盖较好的地区如浙江北部山区是该地区的主要碳汇,而城市为CO₂的主要排放源。太湖和陆地生态系统对区域内碳循环起到一定的调节作用,减缓区域大气CO₂浓度的升高。此外,局地气象条件如湖陆风对太湖周边地区大气CO₂浓度有显著影响。     

Experimental investigation of the scavenging of gaseous mercury by sea salt aerosol

Sea salt aerosol may be an important sink for reactive gaseous mercury (RGM) in the marine boundary layer, reducing ambient RGM concentrations and transferring the mercury (Hg) to the oceans and coastal ecosystems. The goal of this study was to determine the affinity of gaseous mercury for sea salt aerosol (SSA) by conducting adsorption experiments with sea salt-coated sampling denuders. In the first set of experiments, ambient outdoor air was passed through denuders coated with either KCl, as in the widely accepted method to sample RGM, or with NaCl, a primary component of sea salt aerosols. On the one sampling day in which RGM was above the MDL, the NaCl coated denuders removed Hg from the ambient air, equivalent to 87% of the RGM in the air (as determined by KCl denuders). For the second set of experiments HgCl₂ generated in the laboratory was passed through denuders coated with KCl and either NaCl or sea salt. The NaCl denuders collected an average of 99 ± 16% of the mercury that the KCl denuders collected. Newly coated sea salt denuders collected 88 ± 17% of the amount of mercury that the KCl denuders collected, but interestingly the sea salt denuders capacity decreased with repeated use. These experiments demonstrate that HgCl₂, a major component of RGM has a strong affinity for NaCl and sea salt and is therefore likely to be scavenged by SSA. This study adds to the growing evidence that RGM is scavenged by sea salt aerosols and therefore more quickly deposited to the ocean and coastal environment.     

中国大陆黑碳气溶胶排放清单

The detailed high-resolution emission inventory of black carbon (BC) from China in the year 2000 was calculated. The latest fuel consumption data including fossil and biomass fuels, and socio-economic statistics used were obtained from government agencies, mostly at the county level, and some new emission factors (Efs) from local measurements were also used. National and regional summaries of emissions were presented at 0.2°×0.2°resolution. Total BC emission was 1499.4 Gg in 2000, mainly due to the burning of coal and biomass. The BC emission estimated here is higher than those in previous studies, mainly because the emissions from coal burning by rural industries and residences were previously underestimated. More BC aerosols were emitted from eastern China than western China. A strong seasonal dependence was observed for BC emissions, with peaks in January and December and low emissions in July and August; and this seasonality is mainly due to patterns in residential heating and the open burning of crop residues.     

The sources and composition of mercury in Pacific Ocean rain

Here we report measurements of total Hg (Hg_T), reactive Hg (Hg_R), and methylmercury (MMHg) in precipitation from the equatorial Pacific Ocean, collected during a cruise in January and February 1990, and from a mid-continental location in the rural temperate lacustrine northcentral Wisconsin environs. The concentrations of Hg_T (14.4±6.5 pM), Hg_R (8.9±4.5 pM) and MMHg (<50 fM) found in equatorial Pacific rain were less than the average concentrations found in Wisconsin. In general, the results indicate that although particulate Hg is a small fraction of the total atmospheric Hg burden, it is the major contributor to Hg in precipitation. Furthermore, deposition could be an important source of Hg_R to the equatorial Pacific Ocean. In contrast, deposition is not a significant source of MMHg to either the equatorial Pacific Ocean or the remote seepage lakes of Wisconsin. This implies that methylated mercury is formedin situ in these systems.     

Atmospheric Mercury Concentrations from Several Observatory Sites in the Northern Hemisphere

In an effort to investigate both large-scale (spatial) and short/long-term (temporal) distribution characteristics of atmospheric mercury, we have combined and analyzed the Hg concentration data sets collected continuously by four different scientific groups for the areas and periods covering (1) America (three sites near the Canadian Great Lakes (CGL): 1997–2000), (2) Asia (Seoul, Korea (SEL): 1997–2002), (3) Arctic (Alert, Canada (ALT): 1995–2001), and (4) Europe (Mace Head, Ireland (MH): 1996–2002). The mean concentrations of Hg data from those widely dispersed monitoring stations were computed to be (1) 1.58 ± 0.23, 1.69 ± 0.32, and 1.93 ± 0.44 (three sites in CGL), (2) 5.06 ± 2.46 ng m^–3 (SEL), (3) 1.55 ± 0.41 (ALT), and (4) 1.76 ± 0.31 (MH). Intersite relationships were investigated among all different stations using the data groups divided into different temporal intervals. The analysis of diurnal variation patterns of Hg indicated differences in regional source/sink characteristics, with increasing amplitudes of variability toward areas under the strong influence of anthropogenic sources. When the analysis was made over different seasons, the patterns contrasted greatly between the Arctic and the other areas. It was found that the relative enhancement of Hg concentrations was dominant during winter/spring in most areas due to direct or indirect influences of anthropogenic emissions. However, the pattern for the Arctic area was distinguished pronouncedly from others with the spring minimum and summer maximum both of which reflect the potent effects of mercury depletion phenomenon (MDP). By contrast, no long-term trend, either being an increase or decrease, was evident from any of the stations during each respective study period. Although our initial attempts to examine the distribution characteristics of Hg analyzed by different scientific groups were successful, we feel that these efforts should be continued further to extend the compatibility of the global database of Hg.     

全球2℃温升碳约束下中国煤电搁浅资产研究

作为全球煤电装机规模最大且仍在扩张的国家,中国需要慎重评估兑现《巴黎协定》温室气体减排承诺带来的潜在煤电资产搁浅问题.研究运用"上下交互"的碳锁定曲线模型,识别不同产能扩张情景下(无新增、新增200、300和400 GW)的搁浅煤电机组.首先,从"自上而下"角度匡算中国煤电行业2℃温升目标下的碳配额.然后,从"自下而上...     

Neyman-Scott cluster model for daily rainfall processes in lower extremadura (Spain): Rainfall Generating Mechanisms

Summary A Neyman-Scott cluster model was fitted to the daily rainfall data recorded at the observatory of Badajoz (southwestern Spain) for the period 1901–1990. The data were previously homogenized. The goodness of the fit that indicated the daily rainfall process follows some Rainfall Generating Mechanism (RGM). Having decided on the criteria that a block of rainfall must fulfill to be considered as a RGM, a method was proposed to classify the days that belong to RGMs according to the 500 hPa and the surface topography. In this method each day is characterized by a string of 22 alphanumeric characters. From the subsequent analysis, the structure of the synoptic patterns associated with each RGM was deduced.With 3 Figures     

Distribution,speciation, and budget of atmospheric mercury

Total gaseous mercury (TGM) concentrations over the Atlantic Ocean and over Central Europe were measured repeatedly in the years 1978–1981. The latitudinal TGM distribution showed a pronounced and reproducible interhemispherical difference with higher TGM concentrations in the Northern Hemisphere. TGM was found to be vertically well mixed within the troposphere. The TGM concentration seems to increase with time at a rate of 10±8%/yr in the Northern and 8±3%/yr in the Southern Hemisphere. Measurements of mercury speciation showed that elemental mercury is the main TGM component contributing more than 92% and 83% of TGM in marine and continental air, respectively. The tropospheric mercury burden was calculated to be 6×10⁹g. The interhemispheric distribution and temporal and spatial variability of TGM imply a tropospheric residence time of TGM of about 1 yr. Sink strengths calculated independently from the measured mercury concentration on particles and in rainwater are consistent with the above figures.     

On the Gas Phase Reactions Between Volatile Biogenic Mercury Species and the Nitrate Radical

Tropospheric mercury is dominated by gas phase species. In this paper, the gas phase reactions between the nitrate radical and volatile biogenic mercury species have been investigated. An upper limit for the gas phase rate coefficient for reaction between elemental mercury and NO₃-radicals was determined to 4 × 10^–15 cm³ molecule^–1 s^–1 by using the fast flow-discharge technique. The reaction between dimethyl mercury and NO₃, previously shown to be rapid, has also been studied in the laboratory with respect to product distribution using FT-IR. The result from the product study is consistent with a transformation of dimethyl mercury into inorganic, divalent mercury. All carbon delivered as dimethyl mercury was transformed into formaldehyde, methanol and methyl peroxynitrate. Hg was observed as a minor (2%) product. By exclusion, HgO is proposed as the mercury-containing product. Thus, the reaction between dimethyl mercury and the nitrate radical is excluded as a source of monomethyl mercury species in the atmosphere.     

中国燃煤电厂碳捕集与生物质掺烧碳捕集改造的经济性

碳捕集与封存（CCS）技术作为解决全球气候变化问题的重要手段之一,能够有效减少CO₂排放。中国作为碳排放大国,当前电力的主要来源仍是煤电,碳捕集（CC）改造在燃煤电厂中有很大的应用潜力。经济性对CC改造的部署至关重要。为此,本文计算了中国各省典型电厂CC改造前后的平准化度电成本,比较了不同省份的CO₂捕集成本与CO₂避免成本,分析了不同掺烧率下生物质掺烧结合碳捕集(bioenergy with carbon capture,BECC)改造的经济性。研究发现,CC改造会导致不同地区的燃煤电厂度电成本增加57.51%~93.38%。煤价较低的华北和西北地区（青海除外）CC改造经济性较好,BECC改造则更适合华中地区。建议在推进燃煤电厂CC和BECC改造时要充分考虑区域资源特点,完善碳市场建设,形成合理碳价以促进CC和BECC部署。     

Diversity of Epiphytic Lichens and Hg Contents of Xanthoria parietina Thalli as Monitors of Geothermal Air Pollution in the Mt. Amiata Area (Central Italy)

The diversity of epiphytic lichens and mercury concentrations in lichen samples were measured to monitor the release of airborne pollutants from the industrial exploitation of geothermal resources in the Mt. Amiata area (Italy). The lichen biodiversity showed a general condition of moderate environmental alteration around the geothermal power plants, contrasting with the low environmental alteration of the remaining sites investigated. According to the accumulated Hg in lichen thalli, it was possible to estimate mean Hg and H₂S concentrations in the air, which resulted in very good agreement with values measured instrumentally. Based on these data and the correlation between lichen diversity values and Hg concentrations in lichens, it was possible to calculate the threshold of 8 μg/m³ H₂S as responsible for the worsening from low to moderate environmental alteration according to the biodiversity of epiphytic lichens, and to infer that around geothermal power plants, although not toxic to humans, H₂S concentrations are such to alter the nasal quality of the air. Based on the growth rate of X. parietina, it was possible to convert Hg concentrations into estimates of average Hg deposition rates, which showed fluxes of the order of 65–100 mg/ha/y, indicating a dispersions factor of about 10⁴ for the Hg emitted from the geothermal power plants.