Continuous measurement of peroxyacetyl nitrate (PAN) in suburban and remote areas of western China

Knowledge on atmospheric abundance of peroxyacetyl nitrate (PAN) is important in assessing the severity of photochemical pollution, and for understanding chemical transformation of reactive odd nitrogen and its impact on the budget of tropospheric ozone (O₃). In summer 2006, continuous measurements of PAN were made using an automatic GC–ECD analyzer with an on-line calibrator at a suburban site of Lanzhou (LZ) and a remote site of Mt. Waliguan (WLG) in western China, with concurrent measurements of O₃, total reactive nitrogen (NO_y) and carbon monoxide (CO). At LZ, several photochemical episodes were observed during the study, and the average mixing ratio of PAN (plus or minus standard deviation) was 0.76 (±0.89) ppbv with the maximum value of 9.13 ppbv, compared to an average value of 0.44 (±0.16) ppbv at remote WLG. The PAN mixing ratios in LZ exhibited strong diurnal variations with a maximum at noon, while enhanced concentrations of PAN were observed in the evening and a minimum in the afternoon at WLG. The daily O₃ and PAN concentration maxima showed a strong correlation (r² = 0.91) in LZ, with a regression slope (PAN/O₃) of 0.091 ppbv ppbv^?1. At WLG, six well-identified pollution plumes (lasting 2–8 h) were observed with elevated concentrations of PAN (and other trace gases), and analysis of backward particle release simulation shows that the high-PAN events at WLG were mostly associated with the transport of air masses that had passed over LZ.     

Measurement of gas-phase total peroxides at the summit of Mount Tai in China

Measurement of ambient gas-phase total peroxides was performed at the summit of Mount Tai (Mt. Tai, 1534 m above sea level) in central-eastern China during March 22–April 24 and June 16–July 20, 2007. The hourly averaged concentration of peroxides was 0.17 ppbv (± 0.16 ppbv, maximum: 1.28 ppbv) and 0.55 ppbv (± 0.67 ppbv, maximum: 3.55 ppbv) in the spring and summer campaigns, respectively. The average concentration of peroxides at Mt. Tai, which is in a heavily polluted region, was much lower than hydrogen peroxide measurements made at some rural mountain sites, suggesting that significant removal processes took place in this region. An examination of diurnal variation and a correlation analysis suggest that these removal processes could include chemical suppression of peroxide production due to the scavenging of peroxy and hydroxy radicals by high NO_x, wet removal by clouds/fogs rich in dissolved sulfur dioxide which reacts quickly with peroxides, and photolysis. These sinks competed with photochemical sources of peroxides, resulting in different mean concentrations and diurnal pattern of peroxides in the spring and summer. A principal component analysis was conducted to quantify the major processes that influenced the variation of peroxide concentrations. This analysis shows that in the spring photochemical production was an important source of peroxides, and the major sink was scavenging during upslope transport of polluted and humid air from the lower part of the planetary boundary layer (PBL) and wet removal by synoptic scale clouds. During the summer, highly polluted PBL air (with high NO_x) was often associated with very low peroxides due to the chemical suppression of HO₂ by high NO_x and wet-removal by clouds/fogs in this sulfur-rich atmosphere, especially during the daytime. Higher concentrations of peroxides, which often appeared at mid-nighttime, were mainly associated with subsidence of air masses containing relatively lower concentrations of NO_y.     

Spatiotemporal modelling of ozone distribution in the State of California

This paper is concerned with the spatiotemporal mapping of monthly 8-h average ozone (O₃) concentrations over California during a 15-years period. The basic methodology of our analysis is based on the spatiotemporal random field (S/TRF) theory. We use a S/TRF decomposition model with a dominant seasonal O₃ component that may change significantly from site to site. O₃ seasonal patterns are estimated and separated from stochastic fluctuations. By means of Bayesian Maximum Entropy (BME) analysis, physically meaningful and sufficiently detailed space–time maps of the seasonal O₃ patterns are generated across space and time. During the summer and winter months the seasonal O₃ concentration maps exhibit clear and progressively changing geographical patterns over time, suggesting the existence of relationships in accordance with the typical physiographic and climatologic features of California. BME mapping accuracy can be superior to that of other techniques commonly used by EPA; its framework can rigorously assimilate useful data sources that were previously unaccounted for; the generated maps offer valuable assessments of the spatiotemporal O₃ patterns that can be helpful in the identification of physical mechanisms and their interrelations, the design of human exposure and population health models, and in risk assessment. As they focus on the seasonal patterns, the maps are not contingent on short-time and locally prevalent weather conditions, which are of no interest in a global and non-forecasting framework. Moreover, the maps offer valuable insight about the space–time O₃ concentration patterns and are, thus, helpful for disentangling the influence of explanatory factors or even for identifying some influential ones that could have been otherwise overlooked.     

China's grazed temperate grasslands are a net source of atmospheric methane

A budget for the methane (CH₄) cycle in the Xilin River basin of Inner Mongolia is presented. The annual CH₄ budget in this region depends primarily on the sum of atmospheric CH₄ uptake by upland soils, emission from small wetlands, and emission from grazing ruminants (sheep, goats, and cattle). Flux rates for these processes were averaged over multiple years with differing summer rainfall. Although uplands constitute the vast majority of land area, they consume much less CH₄ per unit area than is emitted by wetlands and ruminants. Atmospheric CH₄ uptake by upland soils was ?3.3 and ?4.8 kg CH₄ ha^?1 y^?1 in grazed and ungrazed areas, respectively. Average CH₄ emission was 791.0 kg CH₄ ha^?1 y^?1 from wetlands and 8.6 kg CH₄ ha^?1 y^?1 from ruminants. The basin area-weighted average of all three processes was 6.8 kg CH₄ ha^?1 y^?1, indicating that ruminant production has converted this basin to a net source of atmospheric CH₄. The total CH₄ emission from the Xilin River basin was 7.29 Gg CH₄ y^?1. The current grazing intensity is about eightfold higher than that which would result in a net zero CH₄ flux. Since grazing intensity has increased throughout western China, it is likely that ruminant production has converted China's grazed temperate grasslands to a net source of atmospheric CH₄ overall.     

Simulation of global warming potential (GWP) from rice fields in the Tai-Lake region,China by coupling 1:50,000 soil database with DNDC model

Quantifying greenhouse gas (GHG) emissions from wetland ecosystems is a relatively new issue in global climate change studies. China has approximately 22% of the world's rice paddies and 38% of the world's rice production, which are crucial to accurately estimate the global warming potential (GWP) at regional scale. This paper reports an application of a biogeochemical model (DeNitrification and DeComposition or DNDC) for quantifying GWP from rice fields in the Tai-Lake region of China. For this application, DNDC is linked to a 1:50,000 soil database, which was derived from 1107 paddy soil profiles compiled during the Second National Soil Survey of China in the 1980–1990s. The simulated results show that the 2.34 Mha of paddy soil cultivated in rice–wheat rotation in the Tai-Lake region emitted about ?1.48 Tg C, 0.84 Tg N and 5.67 Tg C as CO₂, N₂O, and CH₄ respectively, with a cumulative GWP of 565 Tg CO₂ equivalent from 1982 to 2000. As for soil subgroups, the highest GWP (26,900 kg CO₂ equivalent ha^?1 yr^?1) was linked to gleyed paddy soils accounting for about 4.4% of the total area of paddy soils. The lowest GWP (5370 kg CO₂ equivalent ha^?1 yr^?1) was associated with submergenic paddy soils accounting for about 0.32% of the total area of paddy soils. The most common soil in the area was hydromorphic paddy soils, which accounted for about 53% of the total area of paddy soils with a GWP of 12,300 kg CO₂ equivalent ha^?1 yr^?1. On a regional basis, the annual averaged GWP in the polder, Tai-Lake plain, and alluvial plain soil regions was distinctly higher than that in the low mountainous and Hilly soil regions. As for administrative areas, the average annual GWP of counties in Shanghai city was high. Conversely, the average annual GWP of counties in Jiangsu province was low. The high variability in soil properties throughout the Tai-Lake region is important and affects the net greenhouse gas emissions. Therefore, the use of detailed soil data sets with high-resolution digital soil maps is essential to improve the accuracy of GWP estimates with process-based models at regional and national scales.     

Analysis of cloud and precipitation chemistry at Whiteface Mountain,NY

Federal and state programs over the past two decades have resulted in the reduction of emissions of precursors of acid rain. Concomitant with these changes, measured concentrations of acidity in precipitation and in watersheds have shown a downward trend or improvement. However, another pathway for these precursors is through cloud and fog events that often tend to occur at high-elevation regions affecting the fauna and flora as well. In this study we report on long-term measurements of cloud water and precipitation chemistry made from 1994 onwards at a high-elevation location, Whiteface Mountain NY, in the northeastern United States. Trends and inter-relationship between the ions were examined along with ambient SO₂ measurements and Adirondack lakes chemistry data.     

Night-time radical chemistry during the TORCH campaign

We present one of the most comprehensive studies of night-time radical chemistry to date, from the Tropospheric ORganic CHemistry experiment (TORCH) in the summer of 2003. TORCH provided a wealth of measurements with which to study the oxidizing capacity of the atmosphere. The measurements provided input to a zero-dimensional box model which has been used to study night-time radical chemistry during the campaign. Average night-time predicted concentrations of OH (2.6 × 10⁵ molecule cm^?3), HO₂ (2.9 × 10⁷ molecule cm^?3) and [HO₂+ΣRO₂] radicals (2.2 × 10⁸ molecule cm^?3) were an order of magnitude smaller than those predicted during the daytime. The model under-predicted the night-time measurements of OH, HO₂ and [HO₂+ΣRO₂] radicals, on average by 41%, 16% and 8% respectively. Whilst the model captured the broad features of night-time radical behaviour, some of the specific features that were observed are hard to explain. A rate of radical production assessment was carried out for the whole campaign between the hours of 00:00 and 04:00. Whilst radical production was limited owing to the absence of photolytic reactions, production routes via the reactions of alkenes with O₃ provided an effective night-time radical source. Nitrate radical concentrations were predicted to be 0.6 ppt on average with a peak of 18 ppt on August 9th during a polluted heat wave period. Overall, the nitrate radical contributes about a third of the total initiation via RO₂, mostly through reaction with alkenes.     

Carbon isotope analysis for source identification of atmospheric formaldehyde and acetaldehyde in Dinghushan Biosphere Reserve in South China

Formaldehyde and acetaldehyde are two most abundant carbonyls in ambient air. Biogenic emission has been proposed as a significant source other than anthropogenic emissions and atmospheric secondary formation. Here at a forest site in South China, the carbon isotopic compositions of formaldehyde and acetaldehyde emitted from leaves of three tree species (Litsea rotundifolia, Canarium album and Castanea henryi) were measured in comparison with the bulk carbon isotopic compositions of tree leaves. δ¹³C data of the emitted aldehydes (from ?31‰ to ?46‰) were quite different for tree species, which were all more depleted in ¹³C than the tree-leaf bulk δ¹³C values (from ?27‰ to ?32‰). Formaldehyde in ambient air at the forest site had δ¹³C values different from those of leaf-emitted formaldehyde, indicating other sources for ambient formaldehyde apart from direct emission from leaves, most probably the photooxidation of biogenic hydrocarbon like isoprene and monoterpene. The δ¹³C differences of acetaldehyde between ambient data and those of tree leaves emission were less than 1‰, implying direct biogenic emission as the dominant source.     

Characterization of PM2.5-bound polycyclic aromatic hydrocarbons in Atlanta—Seasonal variations at urban,suburban, and rural ambient air monitoring sites

Twenty-eight polycyclic aromatic hydrocarbons (PAH) and methylated PAHs (Me-PAH) were measured in daily PM_2.5 samples collected at an urban site, a suburban site, and a rural site in and near Atlanta during 2004 (5 samples/month/site). The suburban site, located near a major highway, had higher PM_2.5-bound PAH concentrations than did the urban site, and the rural site had the lowest PAH levels. Monthly variations are described for concentrations of total PAHs (∑PAHs) and individual PAHs. PAH concentrations were much higher in cold months than in warm months, with average monthly ∑PAH concentrations at the urban and suburban-highway monitoring sites ranging from 2.12 to 6.85 ng m^?3 during January–February and November–December 2004, compared to 0.38–0.98 ng m^?3 during May–September 2004. ∑PAH concentrations were found to be well correlated with PM_2.5 and organic carbon (OC) within seasons, and the fractions of PAHs in PM_2.5 and OC were higher in winter than in summer. Methyl phenanthrenes were present at higher levels than their un-substituted homologue (phenanthrene), suggesting a petrogenic (unburned petroleum products) input. Retene, a proposed tracer for biomass burning, peaked in March, the month with the highest acreage and frequency of prescribed burning and unplanned fires, and in December, during the high residential wood-burning season, indicating that retene might be a good marker for burning of all biomass materials. In contrast, potassium peaked only in December, indicating that it might be a more specific tracer for wood-burning.     

The Value of Linking Mitigation and Adaptation: A Case Study of Bangladesh

There are two principal strategies for managing climate change risks: mitigation and adaptation. Until recently, mitigation and adaptation have been considered separately in both climate change science and policy. Mitigation has been treated as an issue for developed countries, which hold the greatest responsibility for climate change, while adaptation is seen as a priority for the South, where mitigative capacity is low and vulnerability is high. This conceptual divide has hindered progress against the achievement of the fundamental sustainable development challenges of climate change. Recent attention to exploring the synergies between mitigation and adaptation suggests that an integrated approach could go some way to bridging the gap between the development and adaptation priorities of the South and the need to achieve global engagement in mitigation. These issues are explored through a case study analysis of climate change policy and practice in Bangladesh. Using the example of waste-to-compost projects, a mitigation-adaptation-development nexus is demonstrated, as projects contribute to mitigation through reducing methane emissions; adaptation through soil improvement in drought-prone areas; and sustainable development, because poverty is exacerbated when climate change reduces the flows of ecosystem services. Further, linking adaptation to mitigation makes mitigation action more relevant to policymakers in Bangladesh, increasing engagement in the international climate change agenda in preparation for a post-Kyoto global strategy. This case study strengthens the argument that while combining mitigation and adaptation is not a magic bullet for climate policy, synergies, particularly at the project level, can contribute to the sustainable development goals of climate change and are worth exploring.