Estimates of indirect global warming potentials for CH4, CO and NOX

Emissions may affect climate indirectly through chemical interactions in the atmosphere, but quantifications of such effects are difficult and uncertain due to incomplete knowledge and inadequate methods. A preliminary assessment of the climatic impact of changes in tropospheric O₃ and CH₄ in response to various emissions is given. For a 10% increase in the CH₄ emissions the relative increase in concentration has been estimated to be 37% larger. The radiative forcing from enhanced levels of tropospheric O₃ is estimated to 37% of the forcing from changes in CH₄. Inclusion of indirect effects approximately doubles the climatic impact of CH₄ emissions. Emissions of NO_x increase tropospheric O₃, while the levels of CH₄ are reduced. For emissions of NO_x from aircraft, the positive effects via O₃ changes are significantly larger than the negative through changes in CH₄. For NO_x emitted from surface sources, the effects through changes in O₃ and CH₄ are estimated to be of similar magnitude and large uncertainty is connected to the sign of the net effect. Emissions of CO have positive indirect effects on climate through enhanced levels of tropospheric o₃ and increased lifetime of CH₄. These results form the basis for estimates of global warming potentials for sustained step increases in emissions.     

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone

Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH₄ and NO _x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO _x emissions during this period while the contribution of CH₄ to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO _x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO _x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.     

Impact of Non-Methane Hydrocarbons on Tropospheric Chemistry and the Oxidizing Power of the Global Troposphere: 3-Dimensional Modelling Results

The impact of natural and anthropogenicnon-methane hydrocarbons (NMHC) on troposphericchemistry is investigated with the global,three-dimensional chemistry-transport model MOGUNTIA.This meteorologically simplified model allows theinclusion of a rather detailed scheme to describeNMHC oxidation chemistry. Comparing model resultscalculated with and without NMHC oxidation chemistryindicates that NMHC oxidation adds 40–60% to surfacecarbon monoxide (CO) levels over the continents andslightly less over the oceans. Free tropospheric COlevels increase by 30–60%. The overall yield of COfrom the NMHC mixture considered is calculated to beabout 0.4 CO per C atom. Organic nitrate formationduring NMHC oxidation, and their transport anddecomposition affect the global distribution of NO _x and thereby O₃ production. The impact of theshort-lived NMHC extends over the entire tropospheredue to the formation of longer-lived intermediateslike CO, and various carbonyl and carboxyl compounds.NMHC oxidation almost doubles the net photochemicalproduction of O₃ in the troposphere and leads to20–80% higher O₃ concentration inNO _x -rich boundarylayers, with highest increases over and downwind ofthe industrial and biomass burning regions. Anincrease by 20–30% is calculated for the remotemarine atmosphere. At higher altitudes, smaller, butstill significant increases, in O₃ concentrationsbetween 10 and 60% are calculated, maximizing in thetropics. NO from lightning also enhances the netchemical production of O₃ by about 30%, leading to asimilar increase in the global mean OH radicalconcentration. NMHC oxidation decreases the OH radicalconcentrations in the continental boundary layer withlarge NMHC emissions by up to 20–60%. In the marineboundary layer (MBL) OH levels can increase in someregions by 10–20% depending on season and NO _x levels.However, in most of the MBL OH will decrease by10–20% due to the increase in CO levels by NMHCoxidation chemistry. The large decreases especiallyover the continents strongly reduce the markedcontrasts in OHconcentrations between land and oceanwhich are calculated when only the backgroundchemistry is considered. In the middle troposphere, OHconcentrations are reduced by about 15%, although dueto the growth in CO. The overall effect of thesechanges on the tropospheric lifetime of CH₄ is a 15%increase from 6.5 to 7.4 years. Biogenic hydrocarbonsdominate the impact of NMHC on global troposphericchemistry. Convection of hydrocarbon oxidationproducts: hydrogen peroxides and carbonyl compounds,especially acetone, is the main source of HO _x in theupper troposphere. Convective transport and additionof NO from lightning are important for the O₃ budgetin the free troposphere.     

NUMERICAL SIMULATION OF ATMOSPHERIC METHANE TRENDS OVER THE LAST 150 YEARS*

A global two-dimensional chemistry model is developed to study long-term trends of CH₄ since industrial revolution.The sources of CH₄,CO and NO_x 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.     

青藏高原闪电与NO_2的分析及中国内陆地区LNO_x产量的估算

为了进一步认识闪电活动与对流层氮氧化物的关系及更准确地估算中国地区闪电产生的氮氧化物(LNOx)总量,选取人口稀疏,工业生产水平较低的青藏高原地区作为研究区域,基于LIS(Lightning Imaging Sensor)和GOME-2(The Global Ozone Monitoring Experiment-2)卫星探测仪资料,分析了青藏高原中部区域2009年1月至2012年2月闪电与对流层NO2垂直浓度(VCD)月均值资料的时空分布特性和相关性。在此基础上,结合Beirle et al.(2004)的LNOx估算方法,估算了中国内陆地区的LNOx产量。结果表明:青藏高原地区对流层NO2与闪电与在年际趋势、空间分布及季节变化上保持很好的一致性,闪电密度与NO2VCD的线性拟合相关系数为0.84,这表明青藏高原地区NOx受人为源影响小,是研究LNOx的理想区域。基于拟合结果,估算得到中国内陆地区LNOx的年均产量为0.15(0.03~0.38)Tg(N)a-1。这一结论进一步缩小了以往研究中中国地区LNOx产量估算的不确定范围,有助于更清楚地认识闪电在中国气候变化中的重要作用。     

Radiative forcing from surface NO x emissions: spatial and seasonal variations

The global three-dimensional Lagrangian chemistry-transport model STOCHEM has been used to follow changes in the tropospheric distributions of methane CH₄ and ozone O₃ following the emission of pulses of the oxides of nitrogen NO _x . Month-long emission pulses of NO _x produce deficits in CH₄ mixing ratios that bring about negative radiative forcing (climate cooling) and decay away with e-folding times of 10–15 years. They also produce short-term excesses in O₃ mixing ratios that bring about positive radiative forcing (climate warming) that decay over several months to produce deficits, with their attendant negative radiative forcing (climate cooling) that decays away in step with the CH₄ deficits. Total time-integrated net radiative forcing is markedly influenced by cancellation between the negative CH₄ and long-term O₃ contributions and the positive short-term O₃ contribution to leave a small negative residual. Consequently, total net radiative forcing from NO _x emission pulses and the global warming potentials derived from them, show a strong dependence on the magnitudes, locations and seasons of the emissions. These dependences are illustrated using the Asian continent as an example and demonstrate that there is no simple robust relationship between continental-scale NO _x emissions and globally-integrated radiative forcing. We find that the magnitude of the time-integrated radiative forcing from NO _x -driven CH₄ depletion tends to approach and outweigh that from ozone enhancement, leaving net time-integrated radiative forcings and global warming potentials negative (climate cooling) in contrast to the situation for aircraft NO _x (climate warming). Control of man-made surface NO _x emissions alone may lead to positive radiative forcing (climate warming).     

Analysis of Air Quality in Eastern China and its Interaction with Other Regions of the World

In this study, we used satellite data (GOME and MOPITT) together with a global chemical-transport-model of atmosphere (MOZART-2) to characterize the chemical/aerosol composition over eastern China. We then estimated the effects of local emissions in China on the chemical budgets in other regions of the world. Likewise, we also investigated the effects of air pollution from other regions on the chemical budget over eastern China. The study shows that the column CO and NO _x concentrations are also high in eastern China. The high CO and NO _x concentrations produce modest levels of O₃ concentrations during summer (about 40 to 50 ppbv) and very low O₃ during winter (about 10 to 20 ppbv) in eastern China. The calculated NO₂ column is fairly consistent from the GOME measurement. The calculated CO column is underestimated from the MOPITT measurement. One of the reasons of the underestimation of the predicted CO is due to a fact that the CO emissions were taken without considering the rapid increase of emissions from 1990 to 2000. The calculated surface O₃ is consistent with the measured values, with strong seasonal variations. However, the measurement is very limited, and more measurements in eastern China will be needed. The column NO₂ has a very strong seasonal variation in eastern China, with the highest concentrations during winter and the lowest concentrations during summer. The cause of this seasonal variability is mainly due to the seasonal changes in the chemical loss of NO _x , which is very high in summer and very low during winter. The effects of the local emissions in China and long-range transport from other regions on the chemical distributions in eastern China are studied. The results show that NO _x concentrations in eastern China are mostly caused by the local emissions in China, especially during the winter. The CO concentration over eastern China is from both the local emissions (30% to 40%) and the transport from other regions. Likewise, the CO emissions in China have an important effect on the other regions of the world, but the effect is limited in the northern hemisphere. The local emissions in China also have an important effect on surface O₃ concentrations. During winter, the local emissions reduce the surface O₃ concentrations by 30 to 50%. During summer, the local emissions produce about 50 to 70% of the O₃ concentration in eastern China.     

Trace Gas Measurements Between Moscow and Vladivostok Using the Trans-Siberian Railroad

Using a laboratory wagon traveling along the Trans-Siberian railroad, O₃, NO, NO₂, CO, CH₄, SF₆ and black carbon aerosol have been measured during the summer of 1996. The expedition from Niznij Novgorod (500 km east of Moscow) to Vladivostok (and back to Moscow) has shown the great potential of the train method; here the first results are presented and discussed. A wealth of boundary layer air data was obtained during the over 18000 km travel without serious contamination problems from the electric train itself. The diurnal O₃ cycle peaked generally below 50 nmole/mole, showed the effects of changes in J(NO₂), and often dropped to a few nmole/mole at night time during inversions. Over the vast Siberian lowlands situated between the Ural mountains and the river Yenisey, CH₄ levels were consistently elevated at around 1.95 µmole/mole, which we mainly attribute to wetland emissions. Over eastern Siberia, however, CH₄ levels were generally lower at 1.85 µmole/mole. In contrast, over the west Siberian lowlands, CO levels were relatively low, often reaching values of only 110 nmole/mole, whereas over eastern Siberia CO levels were higher. Very high CO levels were detected over a 2000 km section east of Chita, along the river Amur, which represented an enormous polluted air mass. ¹⁴C analysis performed on several CO samples confirms that the origin was biomass burning. SF₆, which was measured as a general conserved tracer, showed an eastward attenuation from 4.0 to 3.9 pmole/mole, with peaks in a number of places due to local Russian emissions.     

Measurements of trace gases emitted by Australian savanna fires during the 1990 dry season

During 18–23 July 1990, 31 smoke samples were collected from an aircraft flying at low altitudes through the plumes of tropical savanna fires in the Northern Territory, Australia. The excess (above background) mixing ratios of 17 different trace gases including CO₂, CO, CH₄, several non-methane hydrocarbons (NMHC), CH₃CHO, NO _x (– NO + NO₂), NH₃, N₂O, HCN and total unspeciated NMHC and sulphur were measured. Emissionratios relative to excess CO₂ and CO, and emissionfactors relative to the fuel carbon, nitrogen or sulphur content are determined for each measured species. The emission ratios and factors determined here for carbon-based gases, NO _x , and N₂O are in good agreement with those reported from other biomass burning studies. The ammonia data represent the first such measurements from savanna fires, and indicate that NH₃ emissions are more than half the strength of NO _x emissions. The emissions of NO _x , NH₃, N₂O and HCN together represent only 27% of the volatilised fuel N, and are primarily NO _x (16%) and NH₃ (9%). Similarly, only 56% of the volatilised fuel S is accounted for by our measurements of total unspeciated sulphur.     

A numerical model for one‐dimensional simulation of stratospheric chemistry

Abstract

We describe a one‐dimensional (1‐D) numerical model developed to simulate the chemistry of minor constituents in the stratosphere. The model incorporates most of the chemical species presently found in the upper atmosphere and has been used to investigate the effect of increasing chlorofluorocarbon (CFC) emissions on ozone (O₃).

Our calculations confirm previous results that O₃ depletions in the 20–25 km region, the region of the O₃ maximum, are very sensitive to the relative abundances of Cl_x and NO_y in the lower stratosphere for high Cl_x amounts. The individual abundances of lower stratospheric Cl_x and NO_y amounts are very sensitive to upper tropospheric mixing ratios, which, in turn, are determined largely by surface input fluxes and heterogeneous loss processes. Thus the behaviour of column O₃ depletions at high Cl_x levels is greatly affected, albeit indirectly, by tropospheric processes. For high Cl_x levels the O_x flux from the stratosphere to the troposphere is dramatically reduced, leading to a large reduction in tropospheric O₃. Some of the variation between different published 1‐D model results is most likely due to this critical dependence of O₃ depletion on NO_y‐Cl_x ratios.

Model simulations of time‐dependent CFC effects on ozone indicate that if CFCs were to remain at constant 1980 emission rates while N₂O increased at 0.25% a^?1 and CH₄ increased at 1% a^?1, we could expect a 2.2% decrease in total column O₃ (relative to the 1980 atmosphere) by the year 2000. However, if CFC emission rates were to increase by 3% a^?1 (current estimates are 5–6% a^?1), we would predict a depletion of 2.7% by the year 2000. The calculations for times beyond the year 2000 suggest that the effects on total O₃ will begin to accelerate. If methyl chloroform emissions are added at 7% a^?1 (current estimates are 7–9% a^?1) to the above CFC‐N₂O‐CH₄ scenario we calculate total O₃ depletions by the year 2000 that are 41% larger than those calculated without. This suggests that if the emissions of methyl chloroform continue to increase at their present rate then methyl chloroform could have a significant effect upon total O₃.     

Effects of tropical deforestation on global and regional atmospheric chemistry

A major portion of tropospheric photochemistry occurs in the tropics. Deforestation, colonization, and development of tropical rain forest areas could provoke significant changes in emissions of radiatively and photochemically active trace gases. A brief review of studies on trace-gas emissions in pristine and disturbed tropical habitats is followed by an effort to model regional tropospheric chemistry under undisturbed and polluted conditions. Model results suggest that changing emissions could stimulate photochemistry leading to enhanced ozone production and greater mineral acidity in rainfall in colonized agricultural regions. Model results agree with measurements made during the NASA ABLE missions. Under agricultural/pastoral development scenarios, tropical rain forest regions could export greater levels of N₂O, CH₄, CO, and photochemical precursors of NO _y and O₃ to the global atmosphere with implications for climatic warming.     

Responses of the tropospheric ozone and odd hydrogen radicals to column ozone change

The response of tropospheric ozone to a change in solar UV penetration due to perturbation on column ozone depends critically on the tropospheric NO _x (NO+NO₂) concentration. At high NO _x or a polluted area where there is net ozone production, a decrease in column ozone will increase the solar UV penetration to the troposphere and thus increase the tropospheric ozone concentration. However, the opposite will occur, for example, at a remote oceanic area where NO _x is so low that there is net ozone destruction. This finding may have important implication on the interpretation of the long term trend of tropospheric ozone. A change in column ozone will also induce change in tropospheric OH, HO₂, and H₂O₂ concentrations which are major oxidants in the troposphere. Thus, the oxidation capacity and, in turn, the abundances of many reduced gases will be perturbed. Our model calculations show that the change in OH, HO₂, and H₂O₂ concentrations are essentially independent of the NO _x concentration.     

Satellite Measurements of Tropospheric Column O<Subscript>3</Subscript> and NO<Subscript>2</Subscript> in Eastern and Southeastern Asia: Comparison with a Global Model (MOZART-2)

Satellite measurements of tropospheric column O₃ and NO₂ in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O₃ is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO₂ is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O₃ and NO₂ fields. The analysis of the model results show that the industrial emission of NO_x (NO + NO₂) contributes about 50%–80% to tropospheric column NO₂ in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NO_x to tropospheric column O₃ ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NO_x emissions have a small effect on tropospheric O₃ in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NO_x on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.     

Global financial crisis making a V-shaped fluctuation in NO<Subscript>2</Subscript> pollution over the Yangtze River Delta

The Yangtze River Delta (YRD), China’s main cultural and economic center, has become one of the most seriously polluted areas in the world with respect to nitrogen oxides (NO_x), owing to its rapid industrialization and urbanization, as well as substantial coal consumption. On the basis of nitrogen dioxide (NO₂) density data from ozone monitoring instrument (OMI) and ground-based observations, the effects of industrial fluctuations due to the financial crisis on local NO₂ pollution were quantitatively assessed. The results were as follows. (1) A distinct V-shaped fluctuation of major industrial products, thermal generating capacity, electricity consumption, and tropospheric NO₂ densities was associated with the global financial crisis from May 2007 to December 2009, with the largest anomalies 1.5 times more than standard deviations at the height of the crisis period from November 2008 to February 2009. (2) Among all industrial sectors, thermal power plants were mainly responsible for fluctuations in local NO₂ pollution during the crisis period. Thermal generating capacity had its greatest decrease of 12.10% at the height of the crisis compared with that during November 2007–February 2008, leading to local tropospheric NO₂ density decreasing by 16.97%. As the crisis appeased, thermal generating capacity increased by 29.63% from November 2009 to February 2010, and tropospheric NO₂ densities correspondingly increased by 30.07%. (3) Among all industrial sectors in the YRD, the thermal power sector has the greatest coal consumption of about 65.96%. A decline in thermal power of about 10% can induce a decrease of about 30% in NO_x emissions and NO₂ densities, meaning that a relative small fluctuation in industrial production can lead to a large decrease in tropospheric NO₂ densities over industrially developed areas like the YRD region. Since electricity is mainly obtained from local coal-burning thermal plants without NO_x-processing equipment, installing NO_x-removal devices for all thermal power plants is an important and feasible way of controlling local NO_x pollution at present.     

Subsonic aircraft and ozone trends

Growth in subsonic air traffic over the past 20 years has been dramatic, with an annual increase of }6.1% over the decade between 1978 and 1988. Furthermore, aircraft activities in the year 2000 are predicted to be double those of 1990, with a shift towards more high-flying, longhaul subsonics. Aircraft exhaust gases increase the amount of nitrogen oxides (NO _x ) in the upper troposphere/lower stratosphere through injection at cruise altitudes. Given that NO _x is instrumental in tropospheric ozone production and stratospheric ozone destruction, it is important to determine the influence of subsonic aircraft NO _x emissions on levels of atmospheric ozone. This paper describes calculations designed to investigate the impact that subsonic aircraft may already have had on the atmosphere during the 1980s, run in a 2-D chemical-radiative-transport model. The results indicate a significant increase in upper tropospheric ozone over the decade arising from aircraft emissions. However, when comparing model results with observational data, certain discrepancies appear. Lower stratospheric ozone loss over the 1980s does not appear to be greatly altered by the inclusion of aircraft emissions in the model. However, given the trend in greater numbers of long-haul subsonic aircraft, this factor must be considered in any further calculations.     

A budget analysis of NO x column losses over the Korean peninsula

In this study, the chemical and physical losses of nitrogen oxides (NO_x) over the Korean peninsula were discussed in order to better understand the effects of the NO_x losses on the tropospheric NO₂ columns. Initially, it was found that the physical loss processes due to dry and wet depositions had almost negligible impacts on the NO_x loss processes over the Korean peninsula. In contrast, the hourly NO_x chemical column losses were large at ??10¹⁴ molecules cm^?2 h^?1. The amounts of NO_x removed for 1 hour account for approximately 33?C35% of the episode-averaged tropospheric NO₂ columns during summer over the Korean peninsula. The NO_x chemical column loss rates were 24.1?C70.9 times larger than the NO_x physical column loss rates. In a budget analysis of the NO_x chemical column losses, HNO₃ formation via the reaction of OH + NO₂ had the largest contribution toward the NO_x chemical losses (42?C55% during fall and winter seasons; 76?C77% during spring; 92?C93% during summer). Large amounts of NO_x were also removed by heterogeneous nitrate formation via N₂O₅ condensation during the cold seasons (42?C56%) over the Korean peninsula. The columnar NO_x chemical losses took place mainly due to the two chemico-physical reaction processes, and also showed seasonal variations. PAN (Peroxyacetyl Nitrate) is another NO₂ reservoir of potential importance. If the influence of the PAN-related chemistry on the NO_x budget is considered, it can result in an approximate 69% increase in the NO_x chemical column loss during summer. Such increases in the amounts of NO_x removed for 1 hour due to the formation of PAN were equivalent to 56?C58% of the episode-averaged tropospheric NO₂ columns during summer over the Korean peninsula. Such active NO_x chemical losses during summer are another main factor for the tropospheric NO₂ columns exhibiting their smallest values during summer.     

我国甲烷排放情景分析:IPAC模型结果

近期发布的IPCC第六次评估报告再次强调了短寿命期温室气体减排对温升减缓的作用。甲烷是最重要的短寿命期非CO₂温室气体。在各国提出各自新的减排目标之后,针对甲烷减排的行动方案也越来越多。甲烷减排正在成为下一阶段各国和全球合作的重点领域之一。本文在我国碳减排目标下的能源转型基础上,结合其他非能源活动的减排排放源的减排技术选择基础上,利用IPAC模型对未来甲烷的排放情景进行了分析。在模型设定的两个情景分析基础之上,研究发现,到2050年的能源转型可明显减少能源活动的甲烷排放,和2015年相比能源活动的排放可减少67％。和其他行业相比,能源部门的甲烷减排具有更好的协同性。如果考虑进一步减排甲烷,则需要在考虑其他大气污染物减排的基础上,可通过实现天然气的进一步减排来实现。同时其他部门的甲烷减排也具有很大潜力,低甲烷排放情景可以实现到2050年将甲烷排放减少到1 494万吨,和2015年相比全范围排放可减排58％。     

A global model study of natural bromine sources and the effects on tropospheric chemistry using MOZART4

Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr₃, CH₂BrCl, CHBr₂Cl, CHBrCl₂, and CH₂Br₂) and CH₃Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO _x and NO _x . Globally, the impact of bromine chemistry on tropospheric O₃ is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O₃ burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH₃OOH, H₂O₂).     

Ground-Based Atmospheric CO2, CH4, and CO Column Measurements at Golmud in the Qinghai-Tibetan Plateau and Comparisons with TROPOMI/S5P Satellite Observations

Measurements of carbon dioxide(CO₂), methane(CH₄), and carbon monoxide(CO) are of great importance in the Qinghai-Tibetan region, as it is the highest and largest plateau in the world affecting global weather and climate systems. In this study, for the first time, we present CO₂, CH₄, and CO column measurements carried out by a Bruker EM27/SUN Fourier-transform infrared spectrometer(FTIR) at Golmud(36.42°E, 94.91°N, 2808 m) in August 2021. The mean and...     

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.