| 1. |
- Fowler, D., et al.
(författare)
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Atmospheric composition change : Ecosystems-Atmosphere interactions
- 2009
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 43:33, s. 5193-5267
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Forskningsöversikt (refereegranskat)abstract
- Ecosystems and the atmosphere: This review describes the state of understanding the processes involved in the exchange of trace gases and aerosols between the earth's surface and the atmosphere. The gases covered include NO, NO2, HONO, HNO3, NH3, SO2, DMS, Biogenic VOC, O-3, CH4, N2O and particles in the size range 1 nm-10 mu m including organic and inorganic chemical species. The main focus of the review is on the exchange between terrestrial ecosystems, both managed and natural and the atmosphere, although some new developments in ocean-atmosphere exchange are included. The material presented is biased towards the last decade, but includes earlier work, where more recent developments are limited or absent. New methodologies and instrumentation have enabled, if not driven technical advances in measurement. These developments have advanced the process understanding and upscaling of fluxes, especially for particles, VOC and NH3. Examples of these applications include mass spectrometric methods, such as Aerosol Mass Spectrometry (AMS) adapted for field measurement of atmosphere-surface fluxes using micrometeorological methods for chemically resolved aerosols. Also briefly described are some advances in theory and techniques in micrometeorology. For some of the compounds there have been paradigm shifts in approach and application of both techniques and assessment. These include flux measurements over marine surfaces and urban areas using micrometeorological methods and the up-scaling of flux measurements using aircraft and satellite remote sensing. The application of a flux-based approach in assessment of O-3 effects on vegetation at regional scales is an important policy linked development secured through improved quantification of fluxes. The coupling of monitoring, modelling and intensive flux measurement at a continental scale within the NitroEurope network represents a quantum development in the application of research teams to address the underpinning science of reactive nitrogen in the cycling between ecosystems and the atmosphere in Europe. Some important developments of the science have been applied to assist in addressing policy questions, which have been the main driver of the research agenda, while other developments in understanding have not been applied to their wider field especially in chemistry-transport models through deficiencies in obtaining appropriate data to enable application or inertia within the modelling community. The paper identifies applications, gaps and research questions that have remained intractable at least since 2000 within the specialized sections of the paper, and where possible these have been focussed on research questions for the coming decade.
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| 2. |
- Sutton, M. A., et al.
(författare)
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Dynamics of ammonia exchange with cut grassland : Strategy and implementation of the GRAMINAE Integrated Experiment
- 2009
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Ingår i: Biogeosciences. - : Copernicus Publications (on behalf of the European Geosciences Union). - 1726-4170 .- 1726-4189. ; 6:3, s. 309-331
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Tidskriftsartikel (refereegranskat)abstract
- A major international experiment on ammonia (NH3) biosphere-atmosphere exchange was conducted over intensively managed grassland at Braunschweig, Germany. The experimental strategy was developed to allow an integrated analysis of different features of NH3 exchange including: a) quantification of nearby emissions and advection effects, b) estimation of net NH3 fluxes with the canopy by a range of micrometeorological measurements, c) analysis of the sources and sinks of NH3 within the plant canopy, including soils and bioassay measurements, d) comparison of the effects of grassland management options on NH3 fluxes and e) assessment of the interactions of NH3 fluxes with aerosol exchange processes. Additional technical objectives included the inter-comparison of different estimates of sensible and latent heat fluxes, as well as continuous-gradient and Relaxed Eddy Accumulation (REA) systems for NH3 fluxes. The prior analysis established the spatial and temporal design of the experiment, allowing significant synergy between these objectives. The measurements were made at 7 measurement locations, thereby quantifying horizontal and vertical profiles, and covered three phases: a) tall grass canopy prior to cutting (7 days), b) short grass after cutting (7 days) and c) re-growing sward following fertilization with ammonium nitrate (10 days). The sequential management treatments allowed comparison of sources-sinks, advection and aerosol interactions under a wide range of NH3 fluxes. This paper describes the experimental strategy and reports the grassland management history, soils, environmental conditions and air chemistry during the experiment, finally summarizing how the results are coordinated in the accompanying series of papers.
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| 3. |
- Fowler, D., et al.
(författare)
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Effects of global change during the 21st century on the nitrogen cycle
- 2015
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:24, s. 13849-13893
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Forskningsöversikt (refereegranskat)abstract
- The global nitrogen (N) cycle at the beginning of the 21st century has been shown to be strongly influenced by the inputs of reactive nitrogen (N-r) from human activities, including combustion-related NOx, industrial and agricultural N fixation, estimated to be 220 TgNyr(-1) in 2010, which is approximately equal to the sum of biological N fixation in unmanaged terrestrial and marine ecosystems. According to current projections, changes in climate and land use during the 21st century will increase both biological and anthropogenic fixation, bringing the total to approximately 600 TgNyr(-1) by around 2100. The fraction contributed directly by human activities is unlikely to increase substantially if increases in nitrogen use efficiency in agriculture are achieved and control measures on combustion-related emissions implemented. Some N-cycling processes emerge as particularly sensitive to climate change. One of the largest responses to climate in the processing of Nr is the emission to the atmosphere of NH3, which is estimated to increase from 65 TgNyr(-1) in 2008 to 93 TgNyr(-1) in 2100 assuming a change in global surface temperature of 5 degrees C in the absence of increased anthropogenic activity. With changes in emissions in response to increased demand for animal products the combined effect would be to increase NH3 emissions to 135 TgNyr(-1). Another major change is the effect of climate changes on aerosol composition and specifically the increased sublimation of NH4NO3 close to the ground to form HNO3 and NH3 in a warmer climate, which deposit more rapidly to terrestrial surfaces than aerosols. Inorganic aerosols over the polluted regions especially in Europe and North America were dominated by (NH4)(2)SO4 in the 1970s to 1980s, and large reductions in emissions of SO2 have removed most of the SO42- from the atmosphere in these regions. Inorganic aerosols from anthropogenic emissions are now dominated by NH4NO3, a volatile aerosol which contributes substantially to PM10 and human health effects globally as well as eutrophication and climate effects. The volatility of NH4NO3 and rapid dry deposition of the vapour phase dissociation products, HNO3 and NH3, is estimated to be reducing the transport distances, deposition footprints and inter-country exchange of N-r in these regions. There have been important policy initiatives on components of the global N cycle. These have been regional or country-based and have delivered substantial reductions of inputs of Nr to sensitive soils, waters and the atmosphere. To date there have been no attempts to develop a global strategy to regulate human inputs to the nitrogen cycle. However, considering the magnitude of global Nr use, potential future increases, and the very large leakage of Nr in many forms to soils, waters and the atmosphere, international action is required. Current legislation will not deliver the scale of reductions globally for recovery from the effects of Nr deposition on sensitive ecosystems, or a decline in N2O emissions to the global atmosphere. Such changes would require substantial improvements in nitrogen use efficiency across the global economy combined with optimization of transport and food consumption patterns. This would allow reductions in Nr use, inputs to the atmosphere and deposition to sensitive ecosystems. Such changes would offer substantial economic and environmental co-benefits which could help motivate the necessary actions.
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| 4. |
- Fleischer, K., et al.
(författare)
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Low historical nitrogen deposition effect on carbon sequestration in the boreal zone
- 2015
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Ingår i: Journal of Geophysical Research - Biogeosciences. - 2169-8953. ; 120:12, s. 2542-2561
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Tidskriftsartikel (refereegranskat)abstract
- Nitrogen (N) cycle dynamics and N deposition play an important role in determining the terrestrial biosphere's carbon (C) balance. We assess global and biome-specific N deposition effects on C sequestration rates with the dynamic global vegetation model LPJ-GUESS. Modeled CN interactions are evaluated by comparing predictions of the C and CN version of the model with direct observations of C fluxes from 68 forest FLUXNET sites. N limitation on C uptake reduced overestimation of gross primary productivity for boreal evergreen needleleaf forests from 56% to 18%, presenting the greatest improvement among forest types. Relative N deposition effects on C sequestration (dC/dN) in boreal, temperate, and tropical sites ranged from 17 to 26kgCkgN(-1) when modeled at site scale and were reduced to 12-22kgCkgN(-1) at global scale. We find that 19% of the recent (1990-2007) and 24% of the historical global C sink (1900-2006) was driven by N deposition effects. While boreal forests exhibit highest dC/dN, their N deposition-induced C sink was relatively low and is suspected to stay low in the future as no major changes in N deposition rates are expected in the boreal zone. N deposition induced a greater C sink in temperate and tropical forests, while predicted C fluxes and N-induced C sink response in tropical forests were associated with greatest uncertainties. Future work should be directed at improving the ability of LPJ-GUESS and other process-based ecosystem models to reproduce C cycle dynamics in the tropics, facilitated by more benchmarking data sets. Furthermore, efforts should aim to improve understanding and model representations of N availability (e.g., N fixation and organic N uptake), N limitation, P cycle dynamics, and effects of anthropogenic land use and land cover changes.
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| 5. |
- Burkhardt, J., et al.
(författare)
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Modelling the dynamic chemical interactions of atmospheric ammonia with leaf surface wetness in a managed grassland canopy
- 2009
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Ingår i: Biogeosciences. - Göttingen : Copernicus Publications. - 1726-4170 .- 1726-4189. ; 6:1, s. 67-84
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Tidskriftsartikel (refereegranskat)abstract
- Ammonia exchange fluxes between grassland and the atmosphere were modelled on the basis of stomatal compensation points and leaf surface chemistry, and compared with measured fluxes during the GRAMINAE intensive measurement campaign in spring 2000 near Braunschweig, Germany. Leaf wetness and dew chemistry in grassland were measured together with ammonia fluxes and apoplastic NH4+ and H+ concentration, and the data were used to apply, validate and further develop an existing model of leaf surface chemistry and ammonia exchange. Foliar leaf wetness which is known to affect ammonia fluxes may be persistent after the end of rainfall, or sustained by recondensation of water vapour originating from the ground or leaf transpiration, so measured leaf wetness values were included in the model. pH and ammonium concentrations of dew samples collected from grass were compared to modelled values.The measurement period was divided into three phases: a relatively wet phase followed by a dry phase in the first week before the grass was cut, and a second drier week after the cut. While the first two phases were mainly characterised by ammonia deposition and occasional short emission events, regular events of strong ammonia emissions were observed during the post-cut period. A single-layer resistance model including dynamic cuticular and stomatal exchange could describe the fluxes well before the cut, but after the cut the stomatal compensation points needed to numerically match measured fluxes were much higher than the ones measured by bioassays, suggesting another source of ammonia fluxes. Considerably better agreement both in the direction and the size range of fluxes were obtained when a second layer was introduced into the model, to account for the large additional ammonia source inherent in the leaf litter at the bottom of the grass canopy. Therefore, this was found to be a useful extension of the mechanistic dynamic chemistry model by keeping the advantage of requiring relatively little site-specific information.
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| 6. |
- Hertel, O., et al.
(författare)
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Governing processes for reactive nitrogen compounds in the European atmosphere
- 2012
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Ingår i: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 9:12, s. 4921-4954
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Forskningsöversikt (refereegranskat)abstract
- Reactive nitrogen (Nr) compounds have different fates in the atmosphere due to differences in the governing processes of physical transport, deposition and chemical transformation. N r compounds addressed here include reduced nitrogen (NH x : ammonia (NH 3 ) and its reaction product ammonium (NH 4 + )), oxidized nitrogen (NO y : nitrogen monoxide (NO) + nitrogen dioxide (NO 2 ) and their reaction products) as well as organic nitrogen compounds (organic N). Pollution abatement strategies need to take into account the differences in the governing processes of these compounds when assessing their impact on ecosystem services, biodiversity, human health and climate. NO x (NO + NO 2 ) emitted from traffic affects human health in urban areas where the presence of buildings increases the residence time in streets. In urban areas this leads to enhanced exposure of the population to NO x concentrations. NO x emissions generally have little impact on nearby ecosystems because of the small dry deposition rates of NO x . These compounds need to be converted into nitric acid (HNO 3 ) before removal through deposition is efficient. HNO 3 sticks quickly to any surface and is thereby either dry deposited or incorporated into aerosols as nitrate (NO 3 + ). In contrast to NOx compounds, NH 3 has potentially high impacts on ecosystems near the main agricultural sources of NH 3 because of its large ground-level concentrations along with large dry deposition rates. Aerosol phase NH 4 + and NO 3 + contribute significantly to background PM 2.5 and PM 10 (mass of aerosols with an aerodynamic diameter of less than 2.5 and 10 μm, respectively) with an impact on radiation balance as well as potentially on human health. Little is known quantitatively and qualitatively about organic N in the atmosphere, other than that it contributes a significant fraction of wet-deposited N, and is present in both gaseous and particulate forms. Further studies are needed to characterise the sources, air chemistry and removal rates of organic N emissions.
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| 7. |
- Flechard, C. R., et al.
(författare)
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Dry deposition of reactive nitrogen to European ecosystems: a comparison of inferential models across the NitroEurope network
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:6, s. 2703-2728
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Tidskriftsartikel (refereegranskat)abstract
- Inferential models have long been used to determine pollutant dry deposition to ecosystems from measurements of air concentrations and as part of national and regional atmospheric chemistry and transport models, and yet models still suffer very large uncertainties. An inferential network of 55 sites throughout Europe for atmospheric reactive nitrogen (N-r) was established in 2007, providing ambient concentrations of gaseous NH3, NO2, HNO3 and HONO and aerosol NH4+ and NO3- as part of the NitroEurope Integrated Project. Network results providing modelled inorganic Nr dry deposition to the 55 monitoring sites are presented, using four existing dry deposition routines, revealing inter-model differences and providing ensemble average deposition estimates. Dry deposition is generally largest over forests in regions with large ambient NH3 concentrations, exceeding 30-40 kg N ha(-1) yr(-1) over parts of the Netherlands and Belgium, while some remote forests in Scandinavia receive less than 2 kg N ha(-1) yr(-1). Turbulent Nr deposition to short vegetation ecosystems is generally smaller than to forests due to reduced turbulent exchange, but also because NH3 inputs to fertilised, agricultural systems are limited by the presence of a substantial NH3 source in the vegetation, leading to periods of emission as well as deposition. Differences between models reach a factor 2-3 and are often greater than differences between monitoring sites. For soluble Nr gases such as NH3 and HNO3, the non-stomatal pathways are responsible for most of the annual uptake over many surfaces, especially the non-agricultural land uses, but parameterisations of the sink strength vary considerably among models. For aerosol NH4+ and NO3-, discrepancies between theoretical models and field flux measurements lead to much uncertainty in dry deposition rates for fine particles (0.1-0.5 mu m). The validation of inferential models at the ecosystem scale is best achieved by comparison with direct long-term micrometeorological Nr flux measurements, but too few such datasets are available, especially for HNO3 and aerosol NH4+ and NO3-.
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