A determination of the CH4, NO x and CO2 emissions from the Prudhoe Bay,Alaska oil development

In this paper we quantify the CH₄, CO₂ and NO _x emissions during routine operations at a major oil and gas production facility, Prudhoe Bay, Alaska, using the concentrations of combustion by products measured at the NOAA-CMDL observatory at Barrow, Alaska and fuel consumption data from Prudhoe Bay. During the 1989 and 1990 measurement campaigns, 10 periods (called events) were unambiguously identified where surface winds carry the Prudhoe Bay emissions to Barrow (approximately 300 km). The events ranged in duration from 8–48 h and bring ambient air masses containing substantially elevated concentrations of CH₄, CO₂ and NO _y to Barrow. Using the slope of the observed CH₄ vs CO₂ concentrations during the events and the CO₂ emissions based on reported fuel consumption data, we calculate annual CH₄ emissions of (24+/–8)×10³ metric tons from the facility. In a similar manner, the annual NO _x emissions are calculated to be (12+/–4)×10³ metric tons, which is in agreement with an independently determined value. The calculated CH₄ emissions represent the amount released during routine operations including leakage. However this quantity would not include CH₄ released during non-routine operations, such as from venting or gas flaring.     

我国瓦里关山、兴隆温室气体CO2、CH4和N2O的背景浓度

为了研究中国大陆温室性气体CO₂、CH₄和N₂O大气浓度的区域分布和变化特征以及与人类活动的关系,从1995~2000年,先后在青海瓦里关山全球大气基准站（36°18′N,100°54′E,3810 m）及河北中国科学院兴隆天文台（40°24′N,117°30′E, 940 m）,利用不锈钢瓶取样和气相色谱法分析,观测了两地大气中温室气体CO₂、CH₄和N₂O的浓度及其变化情况。结果表明:兴隆和瓦里关山站CO₂、CH₄和N₂O的同期年平均浓度分别为376.7×10-6和373.5×10-6,1886×10-9和1831×10-9,316.7×10-9和314.9×10-9。从1995~2000年,兴隆站CO₂、CH₄和N₂O的年增长率分别为1.95×10-6,9.02×10-9和0.75×10-9。而瓦里关山站从1997~2000年,CO₂、CH₄和N₂O的年增长率分别为1.41×10-6,9.95×10-9和0.82×10-9。两地大气中三种气体的浓度与年增长率与全球同类台站的观测结果接近。同时也在一定程度上反映了各自不同的环境背景特征。     

Effects of temperature rise and increase in CO2 concentration on simulated wheat yields in Europe

A crop-growth-simulation model based on SUCROS87 was used to study effects of temperature rise and increase of atmospheric CO₂ concentration on wheat yields in several regions in Europe. The model simulated potential and water-limited crop production (growth with ample supply of nutrients and in the absence of damage by pests, diseases and weeds). Historic daily weather data from 13 sites in Western Europe were used as starting point.For potential production (optimal water) a 3 °C temperature rise led to a yield decline due to a shortening of the growing period on all locations. Doubling of the CO₂ concentration caused an increase in yield of 40% due to higher assimilation rates. It was found that effects of higher temperature and higher CO₂ concentration were nearly additive and the combination of both led to a yield increase of 1–2 ton ha^-1. A very small CO₂-temperature interaction was found: the effect of doubled CO₂ concentration on crop yield was larger at higher temperatures. The inter-annual yield variability was hardly affected.When water was limiting crop-production effects of temperature rise and higher CO₂ levels were different than for the potential production. Rise in temperature led to a smaller yield reduction, doubled CO₂ concentration to a larger yield increase and combination of both led to a large yield increase (3 ton ha^-1) in comparison with yields simulated for the present situation. Both rise in temperature and increase in the CO₂ concentration reduced water requirements of the crop. Water shortages became smaller, leading to a reduction in inter-annual variability. It is concluded that when no major changes in precipitation pattern occur a climate change will not affect wheat yields since negative effects of higher temperatures are compensated by positive effects of CO₂ enrichment.     

Effects of changes in temperature and CO2 concentration on simulated spring wheat yields in The Netherlands

A crop growth simulation model based on SUCROS87 was constructed to study the effects of temperature rise and increase of the atmospheric CO₂ concentration on spring wheat yields in The Netherlands. The model simulated potential production (limited by crop characteristics, temperature and radiation but without any stress from water or nutrient shortages or pests, diseases and weeds) and water-limited production in which growth is also limited by water shortage. The model was validated for the present climatic conditions. When daily weather data from a nearby station were used, the model was well able to simulate yields obtained in field experiments.Effects of several combinations of temperature rise and atmospheric CO₂ concentration on simulated yields were studied. A temperature rise resulted in a reduction in simulated yield due to shortening of the growing period. Large variations existed in the magnitude of this reduction. Increases in atmospheric CO₂ concentration led to yield increases due to higher assimilation rates and to increase of the water use efficiency. Combination of temperature rise and higher CO₂ concentration resulted in small yield increases in years in which water was not limiting growth and large yield increases in dry years.Change of variety or of sowing date could not reduce the negative effects of temperature rise on simulated yields.     

Influence of the surface microlayer on the flux of nonconservative trace gases (CO,H2, CH4, N2O) across the ocean-atmosphere interface

Gas exchange experiments were conducted in the tropical Atlantic Ocean during a ship expedition with FS Meteor using a small rubber raft. The temporal change of the mixing ratios of CO, H₂, CH₄ and N₂O in the headspace of a floating glass box and the concentrations of these gases in the water phase were measured to determine their transfer velocities across the ocean-atmosphere interface. The ocean acted as a sink for these gases when the water was undersaturated with respect to the mixing ratio in the headspace. The transfer velocities were different for the individual gases and showed still large differences even when normalized for diffusivity. Applying the laminar film model, film thicknesses of 20 to 70 m were calculated for the observed flux rates of the different gas species. When the water was supersaturated with respect to atmospheric CO, H₂, CH₄ and N₂O, the transfer velocities of the emission process were smaller than those determined for the deposition process. In case of H₂ and CH₄, emission was even not calculable although, based on the observed gradient, the laminar film model predicted significant fluxes at the air-sea interface. The results are interpreted by destruction processes active within the surface microlayer.     

Effects of high CO2 levels on surface temperature and atmospheric oxidation state of the early Earth

One-dimensional radiative-convective and photochemical models are used to examine the effects of enhanced CO₂ concentrations on the surface temperature of the early Earth and the composition of the prebiotic atmosphere. Carbon dioxide concentrations of the order of 100–1000 times the present level are required to compensate for an expected solar luminosity decrease of 25–30%, if CO₂ and H₂O were the only greenhouse gases present. The primitive stratosphere was cold and dry, with a maximum H₂O volume mixing ratio of 10^–6. The atmospheric oxidation state was controlled by the balance between volcanic emission of reduced gases, photo-stimulated oxidation of dissolved Fe⁺² in the oceans, escape of hydrogen to space, and rainout of H₂O₂ and H₂CO. At high CO₂ levels, production of hydrogen owing to rainout of H₂O₂ would have kept the H₂ mixing ratio above 2×10^–4 and the ground-level O₂ mixing ratio below 10^–11, even if no other sources of hydrogen were present. Increased solar UV fluxes could have led to small changes in the ground-level mixing ratios of both O₂ and H₂.     

Combined effects of elevated [CO2] and high temperature on leaf mineral balance in Coffea spp. plants

Modelling studies predicted that climate change will have strong impacts on the coffee crop, although no information on the effective impact of elevated CO₂ on this plant exists. Here, we aim at providing a first glimpse on the effect of the combined impact of enhanced [CO₂] and high temperature on the leaf mineral content and balance on this important tropical crop. Potted plants from two genotypes of Coffea arabica (cv. Icatu and IPR 108) and one from C. canephora (cv. Conilon Clone 153) were grown under 380 or 700 μL CO₂ L^?1 air, for 1 year, after which were exposed to an stepwise increase in temperature from 25/20 °C (day/night) up to 42/34 °C, over 8 weeks. Leaf macro???(N, P, K, Ca, Mg, S) and micronutrients (B, Cu, Fe, Mn, Zn) concentrations were analyzed at 25/20 °C (control), 31/25 °C, 37/30 °C and 42/34 °C. At the control temperature, the 700 μL L^?1 grown plants showed a moderate dilution effect (between 7 % and 25 %) in CL 153 (for N, Mg, Ca, Fe) and Icatu (for N, K and Fe), but not in IPR 108 (except for Fe) when compared to the 380 μL L^?1 plants. For temperatures higher than control most nutrients tended to increase, frequently presenting maximal contents at 42/34 °C (or 37/30 °C), although the relation between [CO₂] treatments did not appreciably change. Such increases offset the few dilution effects observed under high growth [CO₂] at 25/20 °C. No clear species responses were found considering [CO₂] and temperature impacts, although IPR 108 seemed less sensitive to [CO₂]. Despite the changes promoted by [CO₂] and heat, the large majority of mineral ratios were kept within a range considered adequate, suggesting that this plant can maintain mineral balances in a context of climate changes and global warming.     

大气CO2富集对根际NaCl盐渍的人参果植株干物质生产和水分利用的影响

对单株砂培盆栽的半木质化枝条扦插生根的一月龄人生果（Solanum muricatum Ait.）栽培品种＂Xotus＂,每周浇两次200mL NaCl质量浓度分别为0mg·L-1和25mg·L-1的Hoagland营养液处理2个月,第二个月在控制空气CO2体积分数为（350±10）×10-6、（700±10）×10-6和（1050±10）×10-6的植物生长箱内试验。结果表明,人参果植株干物质生产量和耗水量受根际NaCl盐渍而下降,又随大气CO2升高而增加。根际NaCl盐渍能增大植株叶片蒸腾系数、根/冠比和干物质向枝干和根部分配的比例及积累量,降低根系吸收水分的效率和耗水量。升高大气CO2能促进叶片发育及干物质向地上部其他器官和地下部组织分配,增加总叶面积、比叶干重和各种器官中干物质增长量,提高干物质生产率和水分利用率。根际经25mg·L-1NaCl盐渍处理的植株,总干物质增长量和水分利用率相应下降50%～54%和24%～37%;与350×10-6CO2的处理的植株相比,700×10-6及1050×10-6CO2的处理分别使这两项指标提高到79%～106%和61%～88%以及133%～189%和99%～142%。大气CO2富集能改善受NaCl盐渍的植株干物质生产力、提高水分利用率。根际NaCl盐渍和大气CO2富集对人参果植株干物质生产和水分利用有生物互作效应。它们的共同作用会促进植株干物质的增长及叶片中合成的干物质向其他器官分配,提高干物质生产率和水分利用率,同时减少总叶面积、枝条和根系干重、根系吸水效率、植株耗水量和叶片蒸腾系数。因此,全球大气CO2富集将有利于该作物的干物质生产和水分利用。     

Analysis of variability and diurnal range of daily temperature in a nested regional climate model: comparison with observations and doubled CO2 results

Analysis of daily variability of temperature in climate model experiments is important as a model diagnostic and for determination of how such variability may change under perturbed climate conditions. The latter could be important from a climate impacts perspective. We analyze daily mean, diurnal range and variability of surface air temperature in two continuous 3 1/2 year long climate simulations over the continental USA, one for present day conditions and one for conditions under doubled carbon dioxide concentration, conducted with a regional climate model (RegCM), on a 60 km grid, nested in a general circulation model (GCM). Model output is compared with a 30-year daily observational data set for various regions of the USA. In comparison with observations the diurnal range in the model control run is somewhat too low although the daily temperature mean is often well reproduced. The daily variability of temperature is underestimated by the model in all areas, but particularly when and where the observed variability is relatively high. Causes for these underestimations are traced to deficiencies in the general circulation of the driving GCM. With doubled CO₂, both maximum and minimum temperatures increase, but the change in the diurnal temperature range (DTR) varies spatially and seasonally. On an annual average over the land domain, the DTR decreases by 0.25'C. Changes in DTR are most strongly correlated with changes in absorbed shortwave radiation at the surface, which explains 72% of the variance in DTR on an annual basis. Change in evaporation was a factor affecting DTR only in the summer when it explained 52% of the variance. The most significant findings with CO₂ doubling are substantial decreases in daily variability in winter over large portions of the domain, and localized increases in summer. Causes for these changes are traced to fluctuations in the intensity and position of the jet stream.     

Formulation and Evaluation of IMS, an Interactive Three-Dimensional Tropospheric Chemical Transport Model 2. Model Chemistry and Comparison of Modelled CH4, CO, and O3 with Surface Measurements

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.     

Effect of climate change and increased atmospheric CO2 on hydrological and nitrogen cycling in an intensive agricultural headwater catchment in western France

Climate change and increased atmospheric CO₂ concentration can impact hydrological and nitrogen cycling at the catchment scale. The objective of this study is to assess these impacts in an intensive agricultural headwater catchment in western France. A calibrated and validated agro-hydrological model was driven by output of the climate model ARPEGE under the A1B emission scenario over 30-year simulation periods. Our study indicated that with climate warming and increased atmospheric CO₂, the main trends in water balance were a decrease in annual actual evapotranspiration (AET), a decrease in annual discharge and wetland extent, and a decrease in spring and summer of groundwater recharge and soil-water content. Not considering the effects of increased atmospheric CO₂ in the agro-hydrological model led to overestimating discharge decrease and underestimating AET decrease and wetland extent. Climate change could influence N cycling by increasing soil N mineralisation, increasing soil denitrification in wetlands and upstream areas, and decreasing NO₃–N load to streams. Since wetlands appear to be sensitive to climate change, improving modelling to better predict their responses is an important issue, especially to help plan sustainable management of these vulnerable areas.     

In situ Measurement of H2O and CH4 with Telecommunication Laser Diodes in the Lower Stratosphere: Dehydration and Indication of a Tropical Air Intrusion at Mid-Latitudes

Telecommunication laser diodes emitting near 1.39 m and 1.65 m in combination with direct-differential absorption spectroscopy are efficient tools to monitor in situ stratospheric H₂O andCH₄ with a good precision error (a few percents), a high temporal resolution (ranging from 10 ms to 1 s), a large dynamic range in the concentration measurements (four orders of magnitude) and a high selectivity in the analyte species. To illustrate the capability of laser probing technique, we report balloonborne H₂Oand CH₄ simultaneous measurements obtained on October 2001 atmidlatitudes (43° N). The H₂O vertical profile achieved with the lasersensor in the lower stratosphere is compared with the H₂O data yielded by a balloonborne frost-point hygrometer. The total hydrogen mixing ratio in the lower stratosphere, 2[CH₄] + [H₂O], appears to beconstant at 7.5 ± 0.1 ppmv. Nevertheless, an unexpected largedehydration of 0.5 ppmv was detected by both the laser sensor and thehygrometer between 16 km and 23 km. We suspect the occurrence of a tropicalair intrusion into mid-latitudes. We support this interpretation using a high-resolution advection model for potential vorticity.     

The effect of nitrogen fertilization on the COS and CS2 emissions from temperature forest soils

The net fluxes of carbonyl sulfide (COS) and carbon disulfide (CS₂) to the atmosphere from nitrogen amended and unamended deciduous and coniferous forest soils were measured during the spring of 1986. We found that emissions of these gases from acidic forest soils were substantially increased after nitrogen fertilization. The total (COS+CS₂) emissions were increased by nearly a factor of three in the hardwood stand and were more than doubled in the pine stand. Furthermore, vegetation type appeared to have an influence on which was the dominant sulfur gas released from the forest soils. The added nitrogen caused a dramatic increase in COS emissions from the hardwood stand (a factor of three increase), while CS₂ emissions from this site were not affected. We observed the opposite response in the pine stand; that is, the nitrogen fertilization had no affect on COS emissions, but did stimulate CS₂ emissions (a factor of more than nine increase).     

Influences of Climate Change on the Uptake and Storage of Anthropogenic CO2 in the Global Ocean

A global ocean general circulation model, called LASG/IAP Climate system ocean model (LICOM), is employed to study the influence of climate change on the uptake and storage of anthropogenic CO 2 in the global ocean. Two simulations were made: the control run (RUN1) with the climatological daily mean forcing data, and the climate change run (RUN2) with the interannually varying daily mean forcing data from the NCEP (National Centers for Environmental Prediction) of the US. The results show that the simulated distributions and storages of anthropogenic dissolved inorganic carbon (anDIC) from both runs are consistent with the data-based results. Compared with the data-based results, the simulations generate higher anDIC concentrations in the upper layer and lower storage amount of anDIC between the subsurface and 1000-m depth, especially in RUN1. A comparison of the two runs shows that the interannually varying forcing can enhance the transport of main water masses, so the rate of interior transport of anDIC is increased. The higher transfer rate of anDIC in RUN2 decreases its high concentration in the upper layer and increases its storage amount below the subsurface, which leads to closer distributions of anDIC in RUN2 to the data-based results than in RUN1. The higher transfer rate in RUN2 also induces larger exchange flux than in RUN1. It is estimated that the global oceanic anthropogenic CO 2 uptake was 1.83 and 2.16 Pg C yr 1 in the two runs in 1995, respectively, and as of 1994, the global ocean contained 99 Pg C in RUN1 and 107 Pg C in RUN2 of anDIC, indicating that the model under the interannually varying forcing could take up 8.1% more anthropogenic carbon than the model under the climatological forcing. These values are within the range of other estimates based on observation and model simulation, while the estimates in RUN1 are near the low bound of other works. It is estimated that the variability of root mean square of the global air-sea anthropogenic carbon flux from the simulated monthly mean results of RUN2 with its seasonal cycle and long-term trend removed is 0.1 Pg C yr 1 . The most distinct anomalies appear to be in the tropical Pacific Ocean and the Southern Ocean.     

The equilibrium constant of NO2 with N2O4 and the temperature dependence of the visible spectrum of NO2: A critical review and the implications for measurements of NO2 in the polar stratosphere

Measurements of stratospheric NO₂ by ground-based visible spectrometers rely on laboratory measurements of absorption cross-sections. We review low-temperature laboratory measurements, which disagree by amounts claimed to be significant. Our recalculation of their errors shows that in general disagreements are not significant and that errors in the ratios of cross-sections at low to room temperature are between ±3% and ±8.8%. Of these errors, up to ±3.5% was contributed by errors in the equilibrium constant,K _p, in those measurements where the pressure was above 0.1 mbar.We review measurements and calculations ofK _p, which were accurate to ±5% from 300 to 233 K. Each method was potentially flawed. For example, infrared measurements of the partial pressure of NO₂ ignored the dependence of absorption on total pressure. From thermodynamic theory, formulae forK _pcan be derived from expressions for the variation of heat capacity with temperature. Contrary to common belief, coefficients in the formulae used by spectroscopists were not derived from the thermodynamic quantities. Rather, they were fitted to measurements or to calculations. Hence, they are empirical and it is dangerous to extrapolate below 233 K, the lowest temperature of the measurements.There are no measurements of NO₂ cross-sections below 230 K. Extrapolation of these cross-sections to analysis of measurements of NO₂ at the low temperatures of the Arctic and Antarctic stratosphere is also dangerous. For satisfactory analysis of polar spectra, the NO₂ cross-sections should be measured at temperatures down to 190 K with a relative accuracy of ±1%. This difficult experiment would need a cell of minimum length 32 m whose length can be adjusted. Because their effects are circular, many errors cannot be removed simply. Although circular errors also arise in the measurements ofK _pand of the infrared spectrum, their weights differ from those in the visible spectrum. The optimum experiment might therefore simultaneously measure the visible and infrared spectra andK _p.     

The influence of volcanic, solar and CO2 forcing on the temperatures in the Dalton Minimum (1790–1830): a model study

The Dalton Minimum (1790–1830) was a period with reduced solar irradiance and strong volcanic eruptions. Additionally, the atmospheric CO₂ concentrations started to rise from the background level of previous centuries. In this period most empirical climate reconstructions indicate a minimum in global or hemispheric temperatures. Here, we analyse several simulations starting in 1755 with the coupled atmosphere-ocean model ECHO-G driven by different forcing combinations to investigate which external forcing could have contributed most strongly to the reduced temperatures during the Dalton Minimum. Results indicate that on global and hemispheric scales, the volcanic forcing is largely responsible for the temperature drop in this period, especially during its second half, whereas changes in solar forcing and the increasing atmospheric CO₂ concentrations were of minor importance. At regional scales, especially the extratropical, the impact of volcanic forcing is much less discernible due to the large regional variability, a finding that agrees with empirical temperature reconstructions.     

Local and Global Similarity in Turbulent Transfer of Heat, Water Vapour, And CO 2 in the Dynamic Convective Sublayer Over a Suburban Area

We investigated the ‘local’ and ‘global’ similarity of vertical turbulent transfer of heat, water vapour, and CO₂ within an urban surface layer. The results were derived from field measurements in a residential area of Tokyo, Japan during midday on fair-weather days in July 2001. In this study, correlation coefficients and quadrant analysis were used for the evaluation of ‘global’ similarity and wavelet analysis was employed for investigating ‘local’ similarity. The correlation coefficients indicated that the transfer efficiencies of water vapour and CO₂ were generally smaller than that of heat. Using wavelet analysis, we found that heat is always efficiently transferred by thermal and organized motions. In contrast, water vapour and CO₂, which are passive quantities, were not transferred as efficiently as heat. The quadrant analyses showed that the heat transfer by ejection exceeded that by sweep, and the ratios of ejection to sweep for water vapour and CO₂ transfer were less than that for heat. This indicated that heat is more efficiently transferred by upward motions and supported the findings from wavelet analysis. The differences of turbulent transfer between heat and both CO₂ and water vapour were probably caused both by the active role of temperature and the heterogeneity in the source distribution of scalars