The seasonal cycles and photochemistry of C2–C5 alkanes at Mace Head

Continuous in-situ measurements of NMHCs at Mace Head, Ireland during two full annual cycles from January 2005 to January 2007 were used to investigate NMHC emission sources and transport including dilution and photochemical oxidation. The Mace Head research station is ideally located to sample a wide range of air masses including polluted European transport, clean North Atlantic and Arctic air masses and the ultra-clean, Southern Atlantic air masses. The variety in air mass sampling is used to investigate interaction of emissions, transport, dilution and photochemistry. Variability of long-lived hydrocarbon ratios is used to assess and estimate typical transport times from emission source to the Mace Head receptor. Seasonality in the ratios of isomeric alkane pairs (for butane and pentanes) are used to assess the effects of atmospheric transport and photochemical ageing. Finally, the natural logarithms of NMHC ratios are used to assess photochemical oxidation.     

Influence of boundary conditions on CMAQ simulations over the Iberian Peninsula

The influence of chemical boundary conditions (BC) on the response of the Community Multiscale Air Quality (CMAQ) model over the Iberian Peninsula was investigated in this study. Three strategies to supply boundary conditions in the context of the Integrated Assessment Modelling System for the Iberian Peninsula (SIMCA) were tested. Alternative methods consist in providing BC from (1) fixed, time-independent, concentration profiles, (2) concentrations predicted in a CMAQ mother domain (48 km, 1 h resolution) and (3) concentration values from the GEOS-Chem chemical-transport global model (2 × 2.5°, 3 h resolution). High resolution (3 km) simulated concentrations of the main pollutants (NO₂, NO, SO₂, O₃, PM₁₀ and PM_2.5) were compared through a comprehensive statistical analysis including observational data from 165 monitoring stations all over the Iberian Peninsula. It was found that model sensitivity to BC for nitrogen and sulphur oxides was limited, being restricted to the vicinity of model boundaries. However, significant domain-wide differences were found when modelling ozone and PM depending on the BC provided to run the tests. Although model performance was affected by spatial and seasonal factors, the results indicate that model-derived, dynamic BC improved CMAQ predictions when compared to those based on static concentrations prescribed in the boundaries. Aggregated statistics suggest that the GEOS-Chem produced the best results for O₃ and PM_2.5 while NO₂ and PM₁₀ were slightly better predicted under the CMAQ nesting approach. Besides the statistical evaluation some other relevant issues in the context of Integrated Assessment Modelling (IAM) are discussed to gain a better insight into the suitability of the methods analyzed and limitations of downscaling methods. Despite being useful to get a better understanding of the role of BC in SIMCA, this study contributed to highlight model deficiencies and therefore to point out future research needs to improve IAM activities in the Iberian Peninsula.     

Comprehensive analysis of the carbon impacts of vehicle intelligent speed control

In recent years sophisticated technologies have been developed to control vehicle speed based on the type of road the vehicle is driven on using Global Positioning Systems and in-car technology that can alter the speed of the vehicle. While reducing the speed of road vehicles is primarily of interest from a safety perspective, vehicle speed is also an important determinant of vehicle emissions and thus these technologies can be expected to have impacts on a range of exhaust emissions. This work analyses the results from a very large, comprehensive field trial that used 20 instrumented vehicles with and without speed control driven almost 500,000 km measuring vehicle speed at 10 Hz. We develop individual vehicle modal emissions models for CO₂ for 30 Euro III and Euro IV cars at a 1-Hz time resolution. Generalized Additive Models were used to describe how emissions from individual vehicles vary depending on their driving conditions, taking account of variable interactions and time-lag effects. We quantify the impact that vehicle speed control has on-vehicle emissions of CO₂ by road type, fuel type and driver behaviour. Savings in CO₂ of ≈6% were found on average for motorway-type roads when mandatory speed control was used compared with base case conditions. For most other types of road, speed control has very little effect on emissions of CO₂ and in some cases can result in increased emissions for low-speed limit urban roads. We also find that there is on average a 20% difference in CO₂ emission between the lowest and highest emitting driver, which highlights the importance of driver behaviour in general as a means of reducing emissions of CO₂.     

Assessment of the uncertainty of using an inverse-dispersion technique to measure methane emissions from animals in a barn and in a small pen

Dispersion techniques are useful for assessing the effectiveness of management practices in mitigating methane (CH₄) emissions from animal operations. In this paper, the accuracy of an inverse-dispersion technique was examined for two common situations: 1) emissions from animals in a barn and 2) emissions from animals in a pen. For both situations, the accuracy of emission estimates generally increased with increasing fetch (scaled to barn height, h, or to pen width, X_s) between the source and the concentration measurement. The gas recovery ratio increased from 0.66 at 5 h to 0.93–1.03 at 10 h–25 h for the barn, and decreased from 1.59 at 0 X_s to 0.99 at 5 X_s and from 1.54 at 0 X_s to 1.09 at 5 X_s for the two small pen scenarios, due to the declining sensitivity of the dispersion model to errors in wind complexity and errors in the assumed source configuration. However, the relative uncertainty of the measured concentration increased with fetch due to the decreasing gas concentrations. Hence, improving the accuracy of emission estimates is a compromise between the source configuration sensitivity and the concentration measurement sensitivity. Fetches of about twice the size of the pen and about 10 times the height of the barn are suggested.     

Isotopes as tracers of sources of lead and strontium in aerosols (TSP & PM2.5) in Beijing

Even after its being phased out in gasoline in the late 90s, lead (Pb) is still present at relatively high levels in the atmosphere of Beijing, China (0.10–0.18 μg m^?3). Its origin is subject to debate as several distinct sources may contribute to the observed pollution levels. This study proposes to constrain the origin(s) of Pb and strontium (Sr) in aerosols, by coupling both Pb and Sr isotope systematics. The characterisation of the main pollution sources (road traffic, smelters, metal refining plants, coal combustion, cement factories, and soil erosion) shows that they can unambiguously be discriminated by the multi-isotope approach (²⁰⁶Pb/²⁰⁴Pb and ⁸⁷Sr/⁸⁶Sr). The study of total suspended particulates (TSP) and fine particles (PM_2.5) from Beijing and its vicinity indicates that both size fractions are controlled by the same sources. Lead isotopes indicate that metal refining plants are the major source of atmospheric lead, followed by thermal power stations and other coal combustion processes. The role of this latter source is confirmed by the study of strontium isotopes. Occasionally, emissions from cement plants and/or input from soil alteration are isotopically detectable.     

Chemical mass balance source apportionment for combined PM2.5 measurements from U.S. non-urban and urban long-term networks

The Minnesota Particulate Matter 2.5 (PM_2.5) Source Apportionment Study was undertaken to explore the utility of PM_2.5 mass, element, ion, and carbon measurements from long-term speciation networks for pollution source attribution. Ambient monitoring data at eight sites across the state were retrieved from the archives of the Interagency Monitoring of Protected Visual Environments (IMPROVE) and the Speciation Trends Network (STN; part of the Chemical Speciation Network [CSN]) and analyzed by an Effective Variance – Chemical Mass Balance (EV-CMB) receptor model with region-specific geological source profiles developed in this study. PM_2.5 was apportioned into contributions of fugitive soil dust, calcium-rich dust, taconite (low grade iron ore) dust, road salt, motor vehicle exhaust, biomass burning, coal-fired utility, and secondary aerosol. Secondary sulfate and nitrate contributed strongly (49–71% of PM_2.5) across all sites and was dominant (≥60%) at IMPROVE sites. Vehicle exhausts accounted for 20–70% of the primary PM_2.5 contribution, largely exceeding the proportion in the primary PM_2.5 emission inventory. The diesel exhaust contribution was separable from the gasoline engine exhaust contribution at the STN sites. Higher detection limits for several marker elements in the STN resulted in non-detectable coal-fired boiler contributions which were detected in the IMPROVE data. Despite the different measured variables, analytical methods, and detection limits, EV-CMB results from a nearby IMPROVE-STN non-urban/urban sites showed similar contributions from regional sources – including fugitive dust and secondary aerosol. Seasonal variations of source contributions were examined and extreme PM_2.5 episodes were explained by both local and regional pollution events.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

Several natural and anthropogenic radionuclides (²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of ²¹⁰Pb was 126 Bq m⁻² a⁻¹, very close to the flux of northern hemisphere average (125 Bq m⁻² a⁻¹). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.     

Concentration and characterization of plutonium in soils of Hubei in central China

To study the Pu concentration and isotope ratio distributions present in China, the ^239+240Pu total activities and ²⁴⁰Pu/²³⁹Pu atom ratios in core soil samples from Hubei Province in central China were investigated using Accelerator Mass Spectrometry (AMS). The activities ranged from 0.019 to 0.502 mBq g⁻¹ and the ^239+240Pu inventories of 45 and ∼55 Bq m⁻² agree well with that expected from global fallout. The ²⁴⁰Pu/²³⁹Pu atom ratios in the soil ranged from 0.172 to 0.220. The ratios are similar to typical global fallout values. Hence, any close-in fallout contribution from the Chinese nuclear weapons tests, mainly conducted in the 1970s, must have either been negligible or had a similar ²⁴⁰Pu/²³⁹Pu ratio to that of global fallout. The top 10 cm layer of the soil contributes ∼90% of the total inventory and the maximum concentrations appeared in the 2-4 cm or 4-6 cm layers. It is suggested that climatic conditions and organic content are the two main factors that affect the vertical migration of plutonium in soil.     

Will photosynthetic capacity of aspen trees acclimate after long-term exposure to elevated CO2 and O3?

Photosynthetic acclimation under elevated carbon dioxide (CO₂) and/or ozone (O₃) has been the topic of discussion in many papers recently. We examined whether or not aspen plants grown under elevated CO₂ and/or O₃ will acclimate after 11 years of exposure at the Aspen Face site in Rhinelander, WI, USA. We studied diurnal patterns of instantaneous photosynthetic measurements as well as A/C_i measurements monthly during the 2004-2008 growing seasons. Our results suggest that the responses of two aspen clones differing in O₃ sensitivity showed no evidence of photosynthetic and stomatal acclimation under either elevated CO₂, O₃ or CO₂ + O₃. Both clones 42E and 271 did not show photosynthetic nor stomatal acclimation under elevated CO₂ and O₃ after a decade of exposure. We found that the degree of increase or decrease in the photosynthesis and stomatal conductance varied significantly from day to day and from one season to another.