Natural methyl bromide and methyl chloride emissions from coastal salt marshes

Atmospheric methyl bromide (CH3Br) and methyl chloride (CH3Cl), compounds that are involved in stratospheric ozone depletion, originate from both natural and anthropogenic sources. Current estimates of CH3Br and CH3Cl emissions from oceanic sources, terrestrial plants and fungi, biomass burning and anthropogenic inputs do not balance their losses owing to oxidation by hydroxyl radicals, oceanic degradation, and consumption in soils, suggesting that additional natural terrestrial sources may be important. Here we show that CH3Br and CH3Cl are released to the atmosphere from all vegetation zones of two coastal salt marshes. We see very large fluxes of CH3Br and CH3Cl per unit area: up to 42 and 570 micromol m(-2) d(-1), respectively. The fluxes show large diurnal, seasonal and spatial variabilities, but there is a strong correlation between the fluxes of CH3Br and those of CH3Cl, with an average molar flux ratio of roughly 1:20. If our measurements are typical of salt marshes globally, they suggest that such ecosystems, even though they constitute less than 0.1% of the global surface area, may produce roughly 10% of the total fluxes of atmospheric CH3Br and CH3Cl.     

Halocarbons produced by natural oxidation processes during degradation of organic matter

Volatile halogenated organic compounds (VHOC) play an important role in atmospheric chemical processes-contributing, for example, to stratospheric ozone depletion. For anthropogenic VHOC whose sources are well known, the global atmospheric input can be estimated from industrial production data. Halogenated compounds of natural origin can also contribute significantly to the levels of VHOC in the atmosphere. The oceans have been implicated as one of the main natural sources, where organisms such as macroalgae and microalgae can release large quantities of VHOC to the atmosphere. Some terrestrial sources have also been identified, such as wood-rotting fungi, biomass burning and volcanic emissions. Here we report the identification of a different terrestrial source of naturally occurring VHOC. We find that, in soils and sediments, halide ions can be alkylated during the oxidation of organic matter by an electron acceptor such as Fe(III): sunlight or microbial mediation are not required for these reactions. When the available halide ion is chloride, the reaction products are CH3Cl, C2H5Cl, C3H7Cl and C4H9Cl. (The corresponding alkyl bromides or alkyl iodides are produced when bromide or iodide are present.) Such abiotic processes could make a significant contribution to the budget of the important atmospheric compounds CH3Cl, CH3Br and CH3I.     

不同纬度大气中氯甲烷浓度的研究

氯甲烷在大气中的浓度较低，仅为10^-12级别，用GC－ECD的方法对不同纬度氯甲烷浓度的分析研究表明，大气中氯甲烷的全球浓度表现出从赤道向两级递减的趋势，这种趋势的解释：赤道附近的排放是主要原因。     

不同纬度大气中氯甲烷浓度的研究( 英文)

氯甲烷在大气中的浓度较低 ,仅为 10 -12 级别 .用GC ECD的方法对不同纬度氯甲烷浓度的分析研究表明 ,大气中氯甲烷的全球浓度表现出从赤道向两级递减的趋势 .这种趋势的解释 :赤道附近的排放是主要原因     

Low European methyl chloroform emissions inferred from long-term atmospheric measurements

Methyl chloroform (CH3CCl3, 1,1,1,-trichloroethane) was used widely as a solvent before it was recognized to be an ozone-depleting substance and its phase-out was introduced under the Montreal Protocol. Subsequently, its atmospheric concentration has declined steadily and recent European methyl chloroform consumption and emissions were estimated to be less than 0.1 gigagrams per year. However, data from a short-term tropospheric measurement campaign (EXPORT) indicated that European methyl chloroform emissions could have been over 20 gigagrams in 2000 (ref. 6), almost doubling previously estimated global emissions. Such enhanced emissions would significantly affect results from the CH3CC13 method of deriving global abundances of hydroxyl radicals (OH) (refs 7-12)-the dominant reactive atmospheric chemical for removing trace gases related to air pollution, ozone depletion and the greenhouse effect. Here we use long-term, high-frequency data from Mace Head, Ireland and Jungfraujoch, Switzerland, to infer European methyl chloroform emissions. We find that European emission estimates declined from about 60 gigagrams per year in the mid-1990s to 0.3-1.4 and 1.9-3.4 gigagrams per year in 2000-03, based on Mace Head and Jungfraujoch data, respectively. Our European methyl chloroform emission estimates are therefore higher than calculated from consumption data, but are considerably lower than those derived from the EXPORT campaign in 2000 (ref. 6).     

Strong emission of methyl chloride from tropical plants

Methyl chloride is the largest natural source of ozone-depleting chlorine compounds, and accounts for about 15 per cent of the present atmospheric chlorine content. This contribution was likely to have been relatively greater in pre-industrial times, when additional anthropogenic sources-such as chlorofluorocarbons-were absent. Although it has been shown that there are large emissions of methyl chloride from coastal lands in the tropics, there remains a substantial shortfall in the overall methyl chloride budget. Here we present observations of large emissions of methyl chloride from some common tropical plants (certain types of ferns and Dipterocarpaceae), ranging from 0.1 to 3.7 microg per gram of dry leaf per hour. On the basis of these preliminary measurements, the methyl chloride flux from Dipterocarpaceae in southeast Asia alone is estimated at 0.91 Tg yr-1, which could explain a large portion of missing methyl chloride sources. With continuing tropical deforestation, natural sources of chlorine compounds may accordingly decrease in the future. Conversely, the abundance of massive ferns in the Carboniferous period may have created an atmosphere rich in methyl chloride.     

Atmospheric nitrous oxide observations above the oceanic surface during CHINARE-18

The gas samples in the marine boundary layer were collected from the track for research ship Xuelong during the 18th Chinese Antarctic Research Expedition (CHINARE-18) and nitrous oxide measurements were made by HP5890ECD-GC in the laboratory. The results represent the shipboard N2O data set obtained within the lower troposphere with the average concentration of (313.5±2.6)nL*L-1 from 31°N to 69°S. The results showed a latitudinally weighted, mean interhemispheric difference of 0.61 nL*L-1. The latitudinal distribution of atmospheric N2O concentration was analyzed from northern midlatitudes to Southern Ocean around the Antarctic continent and it was showed that N2O concentration in the current confluences was higher than that in other oceanic areas. This indicated that strong N2O emissions occurred there. The longitudinal distribution of N2O concentrations in the Southern Ocean also showed similar situation. According to the interhemispheric difference of atmospheric N2O concentrations and the two-box model, we estimated that 2/5 of the global flux of N2O into the atmosphere is derived from the sources in the southern hemisphere.     

Intense mixing of lower thermocline water on the crest of the Mid-Atlantic Ridge

Buoyancy exchange between the deep and the upper ocean, which is essential for maintaining global ocean circulation, mainly occurs through turbulent mixing. This mixing is thought to result primarily from instability of the oceanic internal wave field, but internal waves tend to radiate energy away from the regions in which they are generated rather than dissipate it locally as turbulence and the resulting distribution of turbulent mixing remains unknown. Another, more direct, mixing mechanism involves the generation of turbulence as strong flows pass through narrow passages in topography, but the amount of turbulence generated at such locations remains poorly quantified owing to a lack of direct measurements. Here we present observations from the crest of the Mid-Atlantic Ridge in the subtropical North Atlantic Ocean that suggest that passages in rift valleys and ridge-flank canyons provide the most energetic sites for oceanic turbulence. Our measurements show that diffusivities as large as 0.03 m2 s(-1) characterize the mixing downstream of a sill in a well-stratified boundary layer, with mixing levels remaining of the order of 10(-4) m2 s(-1) at the base of the main thermocline. These mixing rates are significantly higher than the diffusivities of the order of 10(-5) m2 s(-1) that characterize much of the global thermocline and the abyssal ocean. Our estimates suggest that overflows associated with narrow passages on the Mid-Atlantic Ridge in the North Atlantic Ocean produce as much buoyancy flux as has previously been estimated for the entire Romanche fracture zone, a large strait in the Mid-Atlantic Ridge that connects the North and South Atlantic basins. This flux is equivalent to the interior mixing that occurs in the entire North Atlantic basin at the depth of the passages, suggesting that turbulence generated in narrow passages on mid-ocean ridges may be important for buoyancy flux at the global scale.     

森林土壤温室气体通量对森林管理和全球大气变化的响应

森林土壤是温室气体重要的源和汇。探讨不同森林管理和全球大气变化下土壤温室气体通量特征,为有效减少温室气体排放及森林可持续管理等提供参考。笔者从森林土壤温室气体(forest soil green house gases)、森林管理(forest mangement)和全球大气变化(global atmospheric change)3个关键研究点,查阅近年来相关研究成果,归纳森林管理和全球大气变化下土壤温室气体通量的一般性模式。CO₂、CH₄和N₂O是3种重要温室气体,其通量间存在协同、消长和随机型耦合关系。森林管理如火烧、采伐和造林等显著影响土壤温室气体通量。一般情况下,火烧导致土壤N₂O通量降低,CH₄吸收量增加,CO₂通量因火烧类型、火烧强度、生态系统类型不同出现增加、减低和无影响3种结果; 采伐通常导致土壤CO₂、CH₄和N₂O排放增加; 造林可使土壤CO₂排放减少,对N₂O和CH₄通量的影响随生态系统类型、造林树种等而改变。全球大气变化如CO₂浓度升高、氮沉降和气温升高影响森林土壤温室气体通量。通常,CO₂浓度升高导致土壤CO₂和N₂O排放量增加,CH₄吸收量降低; 氮沉降促进土壤N₂O排放、抑制CH₄吸收。气温升高导致土壤CO₂和N₂O排放增加。森林管理和全球大气变化对土壤温室气体通量的综合影响是非叠加的,有效的森林管理可能改变土壤温室气体通量对全球大气变化的响应。     

Increased soil emissions of potent greenhouse gases under increased atmospheric CO2

Increasing concentrations of atmospheric carbon dioxide (CO(2)) can affect biotic and abiotic conditions in soil, such as microbial activity and water content. In turn, these changes might be expected to alter the production and consumption of the important greenhouse gases nitrous oxide (N(2)O) and methane (CH(4)) (refs 2, 3). However, studies on fluxes of N(2)O and CH(4) from soil under increased atmospheric CO(2) have not been quantitatively synthesized. Here we show, using meta-analysis, that increased CO(2) (ranging from 463 to 780 parts per million by volume) stimulates both N(2)O emissions from upland soils and CH(4) emissions from rice paddies and natural wetlands. Because enhanced greenhouse-gas emissions add to the radiative forcing of terrestrial ecosystems, these emissions are expected to negate at least 16.6 per cent of the climate change mitigation potential previously predicted from an increase in the terrestrial carbon sink under increased atmospheric CO(2) concentrations. Our results therefore suggest that the capacity of land ecosystems to slow climate warming has been overestimated.     

Importance of rain evaporation and continental convection in the tropical water cycle

Atmospheric moisture cycling is an important aspect of the Earth's climate system, yet the processes determining atmospheric humidity are poorly understood. For example, direct evaporation of rain contributes significantly to the heat and moisture budgets of clouds, but few observations of these processes are available. Similarly, the relative contributions to atmospheric moisture over land from local evaporation and humidity from oceanic sources are uncertain. Lighter isotopes of water vapour preferentially evaporate whereas heavier isotopes preferentially condense and the isotopic composition of ocean water is known. Here we use this information combined with global measurements of the isotopic composition of tropospheric water vapour from the Tropospheric Emission Spectrometer (TES) aboard the Aura spacecraft, to investigate aspects of the atmospheric hydrological cycle that are not well constrained by observations of precipitation or atmospheric vapour content. Our measurements of the isotopic composition of water vapour near tropical clouds suggest that rainfall evaporation contributes significantly to lower troposphere humidity, with typically 20% and up to 50% of rainfall evaporating near convective clouds. Over the tropical continents the isotopic signature of tropospheric water vapour differs significantly from that of precipitation, suggesting that convection of vapour from both oceanic sources and evapotranspiration are the dominant moisture sources. Our measurements allow an assessment of the intensity of the present hydrological cycle and will help identify any future changes as they occur.     

Spatiotemporal variations in mid-upper tropospheric methane over China from satellite observations

Spaceborne measurements by the Atmospheric Infrared Sounder (AIRS) on the EOS/Aqua satellite provide a global view of methane (CH 4 ) distribution in the mid-upper troposphere (MUT-CH 4 ). The focus of this study is to analyze the spatiotemporal varia- tions in MUT-CH 4 over China from 2003 to 2008. Validation of AIRS CH 4 products versus Fourier transform infrared profiles demonstrates that its RMS error is mostly less than 1.5%. A typical atmospheric methane profile is found that shows how concentrations decrease as height increases because of surface emissions. We found that an important feature in the seasonal variation in CH 4 is the two peaks that exist in summer and winter in most parts of China, which is also observed in in-situ measurements at Mt. Waliguan, Qinghai Province, China (36.2879°N 100.8964°E, 3810 m). Also, in the summer, only one peak existed in western and southern China since there are no more significant anthropogenic sources in winter than at any other time of the year. Further analysis of the deseasonalized time-series of AIRS CH 4 in three fixed pressure layers of AIRS from 2003 to 2008 indicates that CH 4 in the Northern Hemisphere has increased abruptly since 2007, with no significant increase occurring before 2007. The increase in China is generally more significant than in other areas around the world, which again correlates with in-situ measurements at Mt. Waliguan.     

碱土金属卤磷酸盐光激励发光材料的研制

本文测定了在X射线辐照下碱土金属卤磷酸盐的光激励谱和光激励发射光谱。研究了助熔剂含量及改变碱土金属卤磷酸盐基质组成对样品的光激励发光强度的影响。找出了Eu~(2+)的最佳含量。确定了碱土金属卤磷酸盐中以Sr_3Ca_2(PO_4)_3Cl:Eu_(0.04)~(2+)的光激励发光最强。     

Increase in observed net carbon dioxide uptake by land and oceans during the past 50 years

One of the greatest sources of uncertainty for future climate predictions is the response of the global carbon cycle to climate change. Although approximately one-half of total CO(2) emissions is at present taken up by combined land and ocean carbon reservoirs, models predict a decline in future carbon uptake by these reservoirs, resulting in a positive carbon-climate feedback. Several recent studies suggest that rates of carbon uptake by the land and ocean have remained constant or declined in recent decades. Other work, however, has called into question the reported decline. Here we use global-scale atmospheric CO(2) measurements, CO(2) emission inventories and their full range of uncertainties to calculate changes in global CO(2) sources and sinks during the past 50 years. Our mass balance analysis shows that net global carbon uptake has increased significantly by about 0.05 billion tonnes of carbon per year and that global carbon uptake doubled, from 2.4?±?0.8 to 5.0?±?0.9 billion tonnes per year, between 1960 and 2010. Therefore, it is very unlikely that both land and ocean carbon sinks have decreased on a global scale. Since 1959, approximately 350 billion tonnes of carbon have been emitted by humans to the atmosphere, of which about 55 per cent has moved into the land and oceans. Thus, identifying the mechanisms and locations responsible for increasing global carbon uptake remains a critical challenge in constraining the modern global carbon budget and predicting future carbon-climate interactions.     

Detection and classification of atmospheric methane oxidizing bacteria in soil

Well-drained non-agricultural soils mediate the oxidation of methane directly from the atmosphere, contributing 5 to 10% towards the global methane sink. Studies of methane oxidation kinetics in soil infer the activity of two methanotrophic populations: one that is only active at high methane concentrations (low affinity) and another that tolerates atmospheric levels of methane (high affinity). The activity of the latter has not been demonstrated by cultured laboratory strains of methanotrophs, leaving the microbiology of methane oxidation at atmospheric concentrations unclear. Here we describe a new pulse-chase experiment using long-term enrichment with 12CH4 followed by short-term exposure to 13CH4 to isotopically label methanotrophs in a soil from a temperate forest. Analysis of labelled phospholipid fatty acids (PLFAs) provided unambiguous evidence of methane assimilation at true atmospheric concentrations (1.8-3.6 p.p.m.v.). High proportions of 13C-labelled C18 fatty acids and the co-occurrence of a labelled, branched C17 fatty acid indicated that a new methanotroph, similar at the PLFA level to known type II methanotrophs, was the predominant soil micro-organism responsible for atmospheric methane oxidation.     

Some advances in atmospheric chemistry

In the recent decade, researches have been carried out by our group on some aspects of atmospheric chemistry through field observation, mechanism analysis and model simulation. Here some main results on greenhouse gas (CH4, N2O) emission from Chinese agricultural fields, aerosol, global carbon cycle and ozone variation in surface laver over China are briefly reported.     

全球地形影响大气和海洋经圈环流的耦合模式研究

利用气候系统模式(CESM1.0)研究陆地地形改变对大气?海洋经圈环流的影响。模式首先给出真实海陆分布及陆地地形情况下的大气?海洋气候态, 然后给出平板陆地情况下(陆地海拔均匀10 m)的气候态。与真实世界相比, 平板陆地情形下大气?海洋经圈环流发生重大改变: 首先, 年平均大气对流中心南移到赤道附近, 使得大气哈德雷环流相对于赤道对称; 其次, 海洋的经向翻转流变强, 大西洋经向翻转流完全消失, 取而代之的是在太平洋出现强大的经向翻转流及热盐环流。在平板陆地情形下, 北半球中高纬度大气抬升减弱, 向北的大气热量输送减少, 北半球温度降低, 大气对流中心因而向赤道迁移; 同时, 海洋向极地的热量输送也减弱, 中高纬度海洋变冷, 北太平洋海水密度增加很多, 北大西洋海水密度降低, 导致海洋经向翻转流从大西洋转移到太平洋。     

Deep convection in the Irminger Sea forced by the Greenland tip jet

Open-ocean deep convection, one of the processes by which deep waters of the world's oceans are formed, is restricted to a small number of locations (for example, the Mediterranean and Labrador seas). Recently, the southwest Irminger Sea has been suggested as an additional location for open-ocean deep convection. The deep water formed in the Irminger Sea has the characteristic temperature and salinity of the water mass that fills the mid-depth North Atlantic Ocean, which had been believed to be formed entirely in the Labrador basin. Here we show that the most likely cause of the convection in the Irminger Sea is a low-level atmospheric jet known as the Greenland tip jet, which forms periodically in the lee of Cape Farewell, Greenland, and is associated with elevated heat flux and strong wind stress curl. Using a history of tip-jet events derived from meteorological land station data and a regional oceanic numerical model, we demonstrate that deep convection can occur in this region when the North Atlantic Oscillation Index is high, which is consistent with observations. This mechanism of convection in the Irminger Sea differs significantly from those known to operate in the Labrador and Mediterranean seas.     

Trend in the atmospheric heat source over the central and eastern Tibetan Plateau during recent decades: Comparison of observations and reanalysis data

The trend in the atmospheric heat source over the central and eastern Tibetan Plateau (CE-TP) is quantitatively estimated using historical observations at 71 meteorological stations, three reanalysis datasets from 1980-2008, and two satellite radiation datasets from 1984-2007. Results show that a weakening of sensible heat (SH) flux over the CE-TP continues. The most significant trend occurs in spring, induced mainly by decelerated surface wind speeds. The ground-air temperature difference shows a notable increasing trend over the last 5 years. Trends in net radiation flux of the atmospheric column over the CE-TP, evaluated by two satellite radiation datasets, are clearly different. Trends in the atmospheric heat source calculated by the three reanalysis datasets are not completely consistent, and even show opposite signals. Results from the two datasets both show a weakening of the heat source but the magnitude of one is significantly stronger, whereas an increase is indicated by the other data. Therefore, it is challenging to accurately calculate the trend in the atmospheric heat source over the CE-TP, particularly from the estimates of the reanalysis datasets.     

Towards robust regional estimates of CO2 sources and sinks using atmospheric transport models

Information about regional carbon sources and sinks can be derived from variations in observed atmospheric CO2 concentrations via inverse modelling with atmospheric tracer transport models. A consensus has not yet been reached regarding the size and distribution of regional carbon fluxes obtained using this approach, partly owing to the use of several different atmospheric transport models. Here we report estimates of surface-atmosphere CO2 fluxes from an intercomparison of atmospheric CO2 inversion models (the TransCom 3 project), which includes 16 transport models and model variants. We find an uptake of CO2 in the southern extratropical ocean less than that estimated from ocean measurements, a result that is not sensitive to transport models or methodological approaches. We also find a northern land carbon sink that is distributed relatively evenly among the continents of the Northern Hemisphere, but these results show some sensitivity to transport differences among models, especially in how they respond to seasonal terrestrial exchange of CO2. Overall, carbon fluxes integrated over latitudinal zones are strongly constrained by observations in the middle to high latitudes. Further significant constraints to our understanding of regional carbon fluxes will therefore require improvements in transport models and expansion of the CO2 observation network within the tropics.