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Combining measurements of atmospheric CO2 and its radiocarbon (14CO2) fraction and transport modeling in atmospheric inversions offers a way to derive improved estimates of CO2 emitted from fossil fuel (FFCO2). In this study, we solve for the monthly FFCO2 emission budgets at regional scale (i.e., the size of a medium-sized country in Europe) and investigate the performance of different observation networks and sampling strategies across Europe. The inversion system is built on the LMDZv4 global transport model at 3.75° ×2.5° resolution. We conduct Observing System Simulation Experiments (OSSEs) and use two types of diagnostics to assess the potential of the observation and inverse modeling frameworks. The first one relies on the theoretical computation of the uncertainty in the estimate of emissions from the inversion, known as "posterior uncertainty", and on the uncertainty reduction compared to the uncertainty in the inventories of these emissions, which are used as a prior knowledge by the inversion (called "prior uncertainty"). The second one is based on comparisons of prior and posterior estimates of the emission to synthetic "true" emissions when these true emissions are used beforehand to generate the synthetic fossil fuel CO2 mixing ratio measurements that are assimilated in the inversion. With 17 stations currently measuring 14CO2 across Europe using 2-week integrated sampling, the uncertainty reduction for monthly FFCO2 emissions in a country where the network is rather dense like Germany, is larger than 30%. With the 43 14CO2 measurement stations planned in Europe, the uncertainty reduction for monthly FFCO2 emissions is increased for the UK, France, Italy, eastern Europe and the Balkans, depending on the configuration of prior uncertainty. Further increasing the number of stations or the sampling frequency improves the uncertainty reduction (up to 40 to 70%) in high emitting regions, but the performance of the inversion remains limited over low-emitting regions, even assuming a dense observation network covering the whole of Europe. This study also shows that both the theoretical uncertainty reduction (and resulting posterior uncertainty) from the inversion and the posterior estimate of emissions itself, for a given prior and "true" estimate of the emissions, are highly sensitive to the choice between two configurations of the prior uncertainty derived from the general estimate by inventory compilers or computations on existing inventories. In particular, when the configuration of the prior uncertainty statistics in the inversion system does not match the difference between these prior and true estimates, the posterior estimate of emissions deviates significantly from the truth. This highlights the difficulty of filtering the targeted signal in the model-data misfit for this specific inversion framework, the need to strongly rely on the prior uncertainty characterization for this and, consequently, the need for improved estimates of the uncertainties in current emission inventories for real applications with actual data. We apply the posterior uncertainty in annual emissions to the problem of detecting a trend of FFCO2, showing that increasing the monitoring period (e.g., more than 20 years) is more efficient than reducing uncertainty in annual emissions by adding stations. The coarse spatial resolution of the atmospheric transport model used in this OSSE (typical of models used for global inversions of natural CO2 fluxes) leads to large representation errors (related to the inability of the transport model to capture the spatial variability of the actual fluxes and mixing ratios at subgrid scales), which is a key limitation of our OSSE setup to improve the accuracy of the monitoring of FFCO2 emissions in European regions. Using a high-resolution transport model should improve the potential to retrieve FFCO2 emissions, and this needs to be investigated. [ABSTRACT FROM AUTHOR]

Atmospheric phosphorus fertilizes plants and contributes to Earth's biogeochemical phosphorus cycle. However, calculations of the global budget of atmospheric phosphorus have been unbalanced, with global deposition exceeding estimated emissions from dust and sea-salt transport, volcanic eruptions, biogenic sources and combustion of fossil fuels, biofuels and biomass, the latter of which thought to contribute about 5% of total emissions. Here we use measurements of the phosphorus content of various fuels and estimates of the partitioning of phosphorus during combustion to calculate phosphorus emissions to the atmosphere from all combustion sources. We estimate combustion-related emissions of 1.8 Tg P yr−1, which represent over 50% of global atmospheric sources of phosphorus. Using these estimates in atmospheric transport model simulations, we find that the total global emissions of atmospheric phosphorus (3.5 Tg P yr−1) translate to a depositional sink of 2.7 Tg P yr−1 over land and 0.8 Tg P yr−1 over the oceans. The modelled spatial patterns of phosphorus deposition agree with observations from globally distributed measurement stations, and indicate a near balance of the phosphorus budget. Our finding suggests that the perturbation of the global phosphorus cycle by anthropogenic emissions is larger thanpreviously thought. [ABSTRACT FROM AUTHOR]

Atmospheric PM10 were measured for 12 months at 18 sites along a 2500 km profile across northern China. Annual mean PM10 concentrations in urban, rural village, and rural field sites were 180 ± 171, 182 ± 154, and 128 ± 89 μg/m3, respectively. The similarities in PM10 concentrations between urban and rural village sites suggest that strong localized emissions and severe contamination in rural residential areas are derived from solid fuels combustion in households. High PM10 concentrations in Wuwei and Taiyuan were caused by either sandstorms or industrial activities. Relatively low PM10 concentrations were observed in coastal areas of Dalian and Yantai. Particulate air pollution was much higher in winter and spring than in summer and fall. Multiple regression analysis indicates that 35% of the total variance can be attributed to sandstorms, precipitation and residential energy consumption. Over 40% of the measurements in both urban and rural village areas exceeded the national ambient air quality standard. [Copyright &y& Elsevier]

The concentration and composition of PAHs emitted from biomass cooking fuel were characterized in a rural non-smoking household in northern China. Twenty-two parent PAHs (pPAHs), 12 nitro-PAHs (nPAHs), and 4 oxy-PAHs (oPAHs) were measured in the kitchen, bedroom, and outdoors during both summer and winter. The most severe contamination occurred in the kitchen in the winter, where the daily mean concentrations of pPAHs, nPAHs, and oPAHs were 7500 ± 4100, 38 ± 29, and 8400 ± 9200 ng/m3, respectively. Our results suggest that the nPAHs were largely from secondary formation in ambient air while oPAHs were either from primary emission of biomass burning or secondary formation from pPAHs in the kitchen. The daily mean benzo(a)pyrene equivalent exposure concentration was as high as 200 ± 160 ng/m3 in the winter for the housewife who did the cooking compared to 59 ± 37 ng/m3 for the control group that did not cook. [Copyright &y& Elsevier]

Bulk deposition samples were collected in remote, rural village and urban areas of Beijing–Tianjin region, North China in spring, summer, fall and winter from 2007 to 2008. The annually averaged PAHs concentration and deposition flux were 11.81 ± 4.61 μg/g and 5.2 ± 3.89 μg/m2/day respectively. PHE and FLA had the highest deposition flux, accounting for 35.3% and 20.7% of total deposition flux, respectively. More exposure risk from deposition existed in the fall for the local inhabitants. In addition, the PAHs deposition flux in rural villages (3.91 μg/m2/day) and urban areas (8.28 μg/m2/day) was 3.8 and 9.1 times higher than in background area (0.82 μg/m2/day), respectively. This spatial variation of deposition fluxes of PAHs was related to the PAHs emission sources, local population density and air concentration of PAHs, and the PAHs emission sources alone can explain 36%, 49%, 21% and 30% of the spatial variation in spring, summer, fall and winter, respectively. [Copyright &y& Elsevier]

Abstract: Residential energy consumptions of both electricity and fuels are associated with emissions of many air pollutants. Temporally and spatially resolved energy consumption data are scarce in China, which are critical for a better understanding of their environmental impacts. In this study, a space-for-time substitution method was proposed and two models for predicting fuel and electricity consumptions in residential sector of China were developed using provincial data. It was found that fuel consumption was not directly proportional to heating degree day and was also affected by heating day, defined as the number of days when heating is required in a year. The models were validated against a set of historical annual data and two sets of survey data on seasonal variations. The models were applied to predict spatial and temporal variations of residential energy consumptions and emissions of various pollutants and to predict net effects of climate warming on energy consumptions and pollutant emissions. The emissions of black carbon (BC), carbon monoxide (CO), and polycyclic aromatic carbons (PAHs) in winter were significantly higher than those in other seasons. For the emissions of carbon dioxide (CO2), sulfur dioxide (SO2), and nitrogen oxides (NO x ), there were two peaks in winter and summer, with the latter increasing gradually over years. It was predicted that per-capita residential energy consumptions would reach 0.43, 0.33, and 0.26toe/cap in 2050 for IPCC scenarios of A1B, B1, and A2, respectively. Climate warming in the future would lead to less residential fuel but more electricity consumptions. Consequently, emissions of BC, CO, and PAHs would decrease mainly in cold climate zones, while emissions of CO2, SO2, and NOx would increase largely in southeast China. [Copyright &y& Elsevier]

In an attempt to reduce uncertainty, global organic carbon (OC) emissions from a total of 70 sources were compiled at 0.1° × 0.1° resolution for 2007 (PKU-OC-2007) and country scale from 1960 to 2009. The compilation took advantage of a new fuel-consumption data product (PKU-Fuel-2007) and a series of newly published emission factors (EF OC ) in developing countries. The estimated OC emissions were 32.9 Tg (24.1–50.6 Tg as interquartile range), of which less than one third was anthropogenic in origin. Uncertainty resulted primarily from variations in EF OC . Asia, Africa, and South America had high emissions mainly because of residential biomass fuel burning or wildfires. Per-person OC emission in rural areas was three times that of urban areas because of the relatively high EF OC of residential solid fuels. Temporal trend of anthropogenic OC emissions depended on rural population, and was influenced primarily by residential crop residue and agricultural waste burning. Both the OC/PM 2.5 ratio and emission intensity, defined as quantity of OC emissions per unit of fuel consumption for all sources, of anthropogenic OC followed a decreasing trend, indicating continuous improvement in combustion efficiency and control measures. [ABSTRACT FROM AUTHOR]

Emission factors (EFs) of parent polycyclic aromatic hydrocarbons (pPAHs), nitrated PAHs (nPAHs), and oxygenated PAHs (oPAHs) were measured for indoor corn straw burned in a brick cooking stove under different burning conditions. The EFs of total 28 pPAHs, 6 nPAHs and 4 oPAHs were (7.9 ± 3.4), (6.5 ± 1.6)×10 −3 , and (6.1 ± 1.4)×10 −1 mg/kg, respectively. Fuel charge size had insignificant influence on the pollutant emissions. Measured EFs increased significantly in a fast burning due to the oxygen deficient atmosphere formed in the stove chamber. In both restricted and enhanced air supply conditions, the EFs of pPAHs, nPAHs and oPAHs were significantly higher than those measured in normal burning conditions. Though EFs varied among different burning conditions, the composition profiles and calculated isomer ratios were similar, without significant differences. The results from the stepwise regression model showed that fuel burning rate, air supply amount, and modified combustion efficiency were the three most significant influencing factors, explaining 72%–85% of the total variations. [ABSTRACT FROM AUTHOR]

Abstract: Biomass pellets are undergoing fast deployment widely in the world, including China. To this stage, there were limited studies on the emissions of various organic pollutants from the burning of those pellets. In addition to parent polycyclic aromatic hydrocarbons, oxygenated PAHs (oPAHs) have been received increased concerns. In this study, emission factors of oPAHs (EFoPAHs) were measured for two types of pellets made from corn straw and pine wood, respectively. Two combustion modes with (mode II) and without (mode I) secondary side air supply in a modern pellet burner were investigated. For the purpose of comparison, EFoPAHs for raw fuels combusted in a traditional cooking stove were also measured. EFoPAHs were 348 ± 305 and 396 ± 387 μg kg−1 in the combustion mode II for pine wood and corn straw pellets, respectively. In mode I, measured EFoPAHs were 77.7 ± 49.4 and 189 ± 118 μg kg−1, respectively. EFs in mode II were higher (2–5 times) than those in mode I mainly due to the decreased combustion temperature under more excess air. Compared to EFoPAHs for raw corn straw and pine wood burned in a traditional cooking stove, total EFoPAHs for the pellets in mode I were significantly lower (p < 0.05), likely due to increased combustion efficiencies and change in fuel properties. However, the difference between raw biomass fuels and the pellets burned in mode II was not statistically significant. Taking both the increased thermal efficiencies and decreased EFs into consideration, substantial reduction in oPAH emission can be expected if the biomass pellets can be extensively used by rural residents. [Copyright &y& Elsevier]

Published emission factors (EFs) often vary significantly, leading to high uncertainties in emission estimations. There are few reliable EFs from field measurements of residential wood combustion in China. In this study, 17 wood fuels and one bamboo were combusted in a typical residential stove in rural China to measure realistic EFs of particulate matter (PM), organic carbon (OC), and elemental carbon (EC), as well as to investigate the influence of fuel properties and combustion conditions on the EFs. Measured EFs of PM, OC, and SC (EFPM, EFOC and EFEC respectively) were in the range of 0.38-6.4, 0.024-3.0, and 0.039-3.9 gJkg (dry basis), with means and standard derivation of 2.2 ± 1.2, 0.62 ± 0.64, and 0.83 ± 0.69 g/kg respectively. Shrubby biomass combustion produced higher EFs than tree woods, and both species had lower EFs than those of indoor crop residue burning (p <005). Significant correlations between EFPM, EFOC, and EFEC were expected. By using a nine-stage cascade impactor, it was shown that size distributions of PM emitted from tree biomass combustions were unimodal with peaks at a diameter less than 0.4 μm (PM0,4), much finer than the PM from indoor crop residue burning. Approximately 79.4% of the total PM from tree wood combustion was PM with a diameter less than 2.1 μm (PM2.1). PM size distributions for shrubby biomasses were slightly different from those for tree fuels. On the basis of the measured EFs, total emissions of PM, OC, and EC from residential wood combustion in rural China in 2007 were estimated at about 303, 75.7, and 92.0 Gg. [ABSTRACT FROM AUTHOR]

Abstract: Forty passive air samplers were deployed to study the occurrence of gas and particulate phase PAHs in remote, rural village and urban areas of Beijing–Tianjin region, North China for four seasons (spring, summer, fall and winter) from 2007 to 2008. The influence of emissions on the spatial distribution pattern of air PAH concentrations was addressed. In addition, the air–soil gas exchange of PAHs was studied using fugacity calculations. The median gaseous and particulate phase PAH concentrations were 222ng/m3 and 114ng/m3, respectively, with a median total PAH concentration of 349ng/m3. Higher PAH concentrations were measured in winter than in other seasons. Air PAH concentrations measured at the rural villages and urban sites in the northern mountain region were significantly lower than those measured at sites in the southern plain during all seasons. However, there was no significant difference in PAH concentrations between the rural villages and urban sites in the northern and southern areas. This urban–rural PAH distribution pattern was related to the location of PAH emission sources and the population distribution. The location of PAH emission sources explained 56%–77% of the spatial variation in ambient air PAH concentrations. The annual median air–soil gas exchange flux of PAHs was 42.2ng/m2/day from soil to air. Among the 15 PAHs measured, acenaphthylene (ACY) and acenaphthene (ACE) contributed to more than half of the total exchange flux. Furthermore, the air–soil gas exchange fluxes of PAHs at the urban sites were higher than those at the remote and rural sites. In summer, more gaseous PAHs volatilized from soil to air because of higher temperatures and increased rainfall. However, in winter, more gaseous PAHs deposited from air to soil due to higher PAH emissions and lower temperatures. The soil TOC concentration had no significant influence on the air–soil gas exchange of PAHs. [Copyright &y& Elsevier]

Abstract: Coal consumption is one important contributor to energy production, and is regarded as one of the most important sources of air pollutants that have considerable impacts on human health and climate change. Emissions of polycyclic aromatic hydrocarbons (PAHs) from coal combustion were studied in a typical stove. Emission factors (EFs) of 16 EPA priority PAHs from tested coals ranged from 6.25 ± 1.16 mg kg−1 (anthracite) to 253 ± 170 mg kg−1 (bituminous), with NAP and PHE dominated in gaseous and particulate phases, respectively. Size distributions of particulate phase PAHs from tested coals showed that they were mostly associated with particulate matter (PM) with size either between 0.7 and 2.1 μm or less than 0.4 μm (PM0.4). In the latter category, not only were more PAHs present in PM0.4, but also contained higher fractions of high molecular weight PAHs. Generally, there were more than 89% of total particulate phase PAHs associated with PM2.5. Gas-particle partitioning of freshly emitted PAHs from residential coal combustions were thought to be mainly controlled by absorption rather than adsorption, which is similar to those from other sources. Besides, the influence of fuel properties and combustion conditions was further investigated by using stepwise regression analysis, which indicated that almost 57 ± 10% of total variations in PAH EFs can be accounted for by moisture and volatile matter content of coal in residential combustion. [ABSTRACT FROM AUTHOR]