Towards a coupled paradigm of NH3 -CO2 biosphere-atmosphere exchange modelling.

Stomatal conductance, one of the major plant physiological controls within NH3 biosphere-atmosphere exchange models, is commonly estimated from semi-empirical multiplicative schemes or simple light- and temperature-response functions. However, due to their inherent parameterization on meteorological proxy variables, instead of a direct measure of stomatal opening, they are unfit for the use in climate change scenarios and of limited value for interpreting field-scale measurements. Alternatives based on H2 O flux measurements suffer from uncertainties in the partitioning of evapotranspiration at humid sites, as well as a potential decoupling of transpiration from stomatal opening in the presence of hygroscopic particles on leaf surfaces. We argue that these problems may be avoided by directly deriving stomatal conductance from CO2 fluxes instead. We reanalysed a data set of NH3 flux measurements based on CO2 -derived stomatal conductance, confirming the hypothesis that the increasing relevance of stomatal exchange with the onset of vegetation activity caused a rapid decrease of observed NH3 deposition velocities. Finally, we argue that developing more mechanistic representations of NH3 biosphere-atmosphere exchange can be of great benefit in many applications. These range from model-based flux partitioning, over deposition monitoring using low-cost samplers and inferential modelling, to a direct response of NH3 exchange to climate change.

Enhanced nitrogen deposition over China.

China is experiencing intense air pollution caused in large part by anthropogenic emissions of reactive nitrogen. These emissions result in the deposition of atmospheric nitrogen (N) in terrestrial and aquatic ecosystems, with implications for human and ecosystem health, greenhouse gas balances and biological diversity. However, information on the magnitude and environmental impact of N deposition in China is limited. Here we use nationwide data sets on bulk N deposition, plant foliar N and crop N uptake (from long-term unfertilized soils) to evaluate N deposition dynamics and their effect on ecosystems across China between 1980 and 2010. We find that the average annual bulk deposition of N increased by approximately 8 kilograms of nitrogen per hectare (P < 0.001) between the 1980s (13.2 kilograms of nitrogen per hectare) and the 2000s (21.1 kilograms of nitrogen per hectare). Nitrogen deposition rates in the industrialized and agriculturally intensified regions of China are as high as the peak levels of deposition in northwestern Europe in the 1980s, before the introduction of mitigation measures. Nitrogen from ammonium (NH4(+)) is the dominant form of N in bulk deposition, but the rate of increase is largest for deposition of N from nitrate (NO3(-)), in agreement with decreased ratios of NH3 to NOx emissions since 1980. We also find that the impact of N deposition on Chinese ecosystems includes significantly increased plant foliar N concentrations in natural and semi-natural (that is, non-agricultural) ecosystems and increased crop N uptake from long-term-unfertilized croplands. China and other economies are facing a continuing challenge to reduce emissions of reactive nitrogen, N deposition and their negative effects on human health and the environment.

How can we possibly resolve the planet's nitrogen dilemma?

Nitrogen is the most crucial element in the production of nutritious feeds and foods. The production of reactive nitrogen by means of fossil fuel has thus far been able to guarantee the protein supply for the world population. Yet, the production and massive use of fertilizer nitrogen constitute a major threat in terms of environmental health and sustainability. It is crucial to promote consumer acceptance and awareness towards proteins produced by highly effective microorganisms, and their potential to replace proteins obtained with poor nitrogen efficiencies from plants and animals. The fact that reactive fertilizer nitrogen, produced by the Haber Bosch process, consumes a significant amount of fossil fuel worldwide is of concern. Moreover, recently, the prices of fossil fuels have increased the cost of reactive nitrogen by a factor of 3 to 5 times, while international policies are fostering the transition towards a more sustainable agro-ecology by reducing mineral fertilizers inputs and increasing organic farming. The combination of these pressures and challenges opens opportunities to use the reactive nitrogen nutrient more carefully. Time has come to effectively recover used nitrogen from secondary resources and to upgrade it to a legal status of fertilizer. Organic nitrogen is a slow-release fertilizer, it has a factor of 2.5 or higher economic value per unit nitrogen as fertilizer and thus adequate technologies to produce it, for instance by implementing photobiological processes, are promising. Finally, it appears wise to start the integration in our overall feed and food supply chains of the exceptional potential of biological nitrogen fixation. Nitrogen produced by the nitrogenase enzyme, either in the soil or in novel biotechnology reactor systems, deserves to have a 'renaissance' in the context of planetary governance in general and the increasing number of people who desire to be fed in a sustainable way in particular.

Disentangling effects of natural and anthropogenic drivers on forest net ecosystem production.

Net Ecosystem Production (NEP) of forests is the net carbon dioxide (CO2) fluxes between land and the atmosphere due to forests' biogeochemical processes. NEP varies with natural drivers such as precipitation, air temperature, solar radiation, plant functional type (PFT), and soil texture, which affect the gross primary production and ecosystem respiration, and thus the net C sequestration. It is also known that deposition of sulphur and nitrogen influences NEP in forest ecosystems. These drivers' respective, unique effects on NEP, however, are often difficult to be individually identified by conventional bivariate analysis. Here we show that by analyzing 22 forest sites with 231 site-year data acquired from FLUXNET database across Europe for the years 2000-2014, the individual, unique effects of these drivers on annual forest CO2 fluxes can be disentangled using Generalized Additive Models (GAM) for nonlinear regression analysis. We show that S and N deposition have substantial impacts on NEP, where S deposition above 5 kg S ha-1 yr-1 can significantly reduce NEP, and N deposition around 22 kg N ha-1 yr-1 has the highest positive effect on NEP. Our results suggest that air quality management of S and N is crucial for maintaining healthy biogeochemical functions of forests to mitigate climate change. Furthermore, the empirical models we developed for estimating NEP of forests can serve as a forest management tool in the context of climate change mitigation. Potential applications include the assessment of forest carbon fluxes in the REDD+ framework of the UNFCCC.

How ammonia feeds and pollutes the world.

It is cheaper to cut ammonia emission now than to deal with its consequences later.

A world of co-benefits: Solving the global nitrogen challenge.

Nitrogen is a critical component of the economy, food security, and planetary health. Many of the world's sustainability targets hinge on global nitrogen solutions, which, in turn, contribute lasting benefits for: (i) world hunger; (ii) soil, air and water quality; (iii) climate change mitigation; and (iv) biodiversity conservation. Balancing the projected rise in agricultural nitrogen demands while achieving these 21st century ideals will require policies to coordinate solutions among technologies, consumer choice, and socioeconomic transformation.

Nitrogen footprints: Regional realities and options to reduce nitrogen loss to the environment.

Nitrogen (N) management presents a sustainability dilemma: N is strongly linked to energy and food production, but excess reactive N causes environmental pollution. The N footprint is an indicator that quantifies reactive N losses to the environment from consumption and production of food and the use of energy. The average per capita N footprint (calculated using the N-Calculator methodology) of ten countries varies from 15 to 47 kg N capita-1 year-1. The major cause of the difference is the protein consumption rates and food production N losses. The food sector dominates all countries' N footprints. Global connections via trade significantly affect the N footprint in countries that rely on imported foods and feeds. The authors present N footprint reduction strategies (e.g., improve N use efficiency, increase N recycling, reduce food waste, shift dietary choices) and identify knowledge gaps (e.g., the N footprint from nonfood goods and soil N process).

PM2.5 pollution is substantially affected by ammonia emissions in China.

Urban air quality in China has been declining substantially in recent years due to severe haze episodes. The reduction of sulfur dioxide (SO2) and nitrogen oxide (NOx) emissions since 2013 does not yet appear to yield substantial benefits for haze mitigation. As the reductions of those key precursors to secondary aerosol formation appears not to sufficient, other crucial factors need to be considered for the design of effective air pollution control strategies. Here we argue that ammonia (NH3) plays a - so far - underestimated role in the formation of secondary inorganic aerosols, a main component of urban fine particulate matter (PM2.5) concentrations in China. By analyzing in situ concentration data observed in major cities alongside gridded emission data obtained from remote sensing and inventories, we find that emissions of NH3 have a more robust association with the spatiotemporal variation of PM2.5 levels than emissions of SO2 and NOx. As a consequence, we argue that urban PM2.5 pollution in China in many locations is substantially affected by NH3 emissions. We highlight that more efforts should be directed to the reduction of NH3 emissions that help mitigate PM2.5 pollution more efficiently than other PM2.5 precursors. Such efforts will yield substantial co-benefits by improving nitrogen use efficiency in farming systems. As a consequence, such integrated strategies would not only improve urban air quality, but also contribute to China's food-security goals, prevent further biodiversity loss, reduce greenhouse gas emissions and lead to economic savings.

Deposition monitoring networks: what monitoring is required to give reasonable estimates of ammonia/ammonium?

Deposition is one of the main loss terms for ammonia and ammonium from the atmosphere. It is also the input for ecosystems that can lead to drastic changes and effects. Deposition networks are needed to evaluate the need and the effect of policies to reduce nitrogen emissions, but also for studying deposition parameters and for developing deposition models. As with ambient concentrations of ammonia, deposition, especially dry deposition, varies strongly in space and in time. Furthermore, the bi-directional surface-atmosphere exchange of ammonia makes the combination of ambient concentration measurements with inferential models inadequate. Developing deposition monitoring networks with reasonable accuracy and representativeness is therefore not straightforward. In Europe several projects have addressed deposition monitoring. From these results it is concluded that a monitoring strategy should consist of a network with a limited amount of super sites combined with a larger number of sites where low cost methods are applied, together with models for generalisation.

Practical considerations for addressing uncertainties in monitoring bulk deposition.

The assessment of the deposition of both wet (rain and cloud) and dry sedimenting particles is a prerequisite for estimating element fluxes in ecosystem research. Many nations and institutions operate deposition networks using different types of sampler. However, these samplers have rarely been characterized with respect to their sink properties. Major errors in assessing bulk deposition can result from poor sampling properties and defective sampling strategies. Relevant properties are: sampler geometry and material, in particular the shape of the rim; sink properties for gases and aerosols; and microbial transformations of the collected samples. An adequate number of replicates allows the identification of samples which are contaminated, in particular by bird droppings. The paper discusses physical and chemical properties of the samplers themselves. The dependence of measurement accuracy on the number of replicates and the sampling area exposed is discussed. Recommendations are given for sampling strategies, and for making corrections and substitution of missing data.

Monitoring and modelling of biosphere/atmosphere exchange of gases and aerosols in Europe.

Monitoring and modelling of deposition of air pollutants is essential to develop and evaluate policies to abate the effects related to air pollution and to determine the losses of pollutants from the atmosphere. Techniques for monitoring wet deposition fluxes are widely applied. A recent intercomparison experiment, however, showed that the uncertainty in wet deposition is relatively high, up to 40%, apart from the fact that most samplers are biased because of a dry deposition contribution. Wet deposition amounts to about 80% of the total deposition in Europe with a range of 10-90% and uncertainty should therefore be decreased. During recent years the monitoring of dry deposition has become possible. Three sites have been operational for 5 years. The data are useful for model development, but also for model evaluation and monitoring of progress in policy. Data show a decline in SO(2) dry deposition, whereas nitrogen deposition remained constant. Furthermore, surface affinities for pollutants changed leading to changes in deposition. Deposition models have been further developed and tested with dry deposition measurements and total deposition measurements on forests as derived from throughfall data. The comparison is reasonable given the measurement uncertainties. Progress in ozone surface exchange modelling and monitoring shows that stomatal uptake can be quantified with reasonable accuracy, but external surface uptake yields highest uncertainty.

Nonlinearities in source receptor relationships for sulfur and nitrogen compounds.

The relationship between emissions and deposition of air pollutants, both spatially and in time forms an important focus for science and for policy makers. In practice, this relationship may become nonlinear if the underlying processes change with time, or in space. Nonlinearities may also appear due to errors in emission or deposition data, and careful scrutiny of both data sources and their relationship provides a means of picking up such deficiencies. Nonlinearities in source receptor relationships for sulfur and nitrogen compounds in Europe have been identified in measurement data for the UK. In the case of sulfur, the dry deposition process has been shown to be strongly influenced by ambient concentrations of NH3, leading to substantial increases in deposition rate as SO2 concentrations decline and the ratio SO2/NH3 decreases. The field evidence extends to measurements over three different surfaces in three countries across Europe. A mechanistic understanding of the cause of this nonlinearity has been provided. Apparent nonlinearities also exist in the sulfur deposition field through the influence of shipping emissions. The effect is clear at west coast locations, where during a period in which land-based sulfur emissions declined by 50%, no significant decline in concentrations of SO(2-) in precipitation were observed. The sites affected are primarily the coastal regions of southwestern UK, where shipping sources contribute a substantial fraction of the deposited sulfur, but the effect is not detectable elsewhere. Full quantification of the spatially disaggregated emission and their changes in time will eliminate this apparent nonlinearity in the source-receptor data. For oxidized nitrogen emission and deposition in the UK, there is strong evidence of nonlinearity in the source-receptor relationship. The concentrations and deposition of NO(3-) in precipitation have declined little following a reduction in emissions of 45% during the period 1987 to 2001. The data imply a significant decrease in the average transport distance for oxidized nitrogen and most probably an increase in the average oxidation rate. However, the net effect of changes in aerosol chemistry due to changes in sulfur emissions and less competition for the main oxidants as a consequence of reductions in sulfur emission have not been separated. A quantitative explanation of the cause of this nonlinearity is lacking and the effects are therefore identified as an important uncertainty for the development of further protocols to control acidification, eutrophication and photochemical oxidants in Europe.

The Dutch N-cascade in the european perspective.

The Netherlands is "well known" for its nitrogen problems; it has one of the highest reactive nitrogen (Nr) emission densities in the world. It is a small country at the delta of several large European rivers. Ever since the industrial revolution, there has been a growing excess of nutrients and related emissions into the atmosphere (ammonia, nitrogen oxides and nitrous oxide) and into groundwater and surface water (nitrate), leading to a large range of cascading environmental impacts. Vehicular traffic, sewage and animal husbandry are the main sources of oxidized and reduced forms of Nr. This paper provides an overview of the origin and fate of nitrogen in the Netherlands, the various reported impacts of nitrogen, the Dutch and European policies to reduce nitrogen emissions and related impacts. In addition, ways are presented to go forward to potentially solve the problems in a European perspective. Solutions include the improvement of nitrogen efficiencies in different systems, technological options and education.

Summary of regulatory/policy/economic issues related to nitrogen.

This is a summary of the two presentations from the session that dealt with the regulatory, policy and economic issues related to nitrogen compounds and the need to reduce their emissions. The papers were presented by Ronald Evans and Jan Willem Erisman. Information on ecological impacts of nitrogen species and atmospheric relationships are presented in other papers in this special issue. This summary provides an overview of the discussions from the above presentations.

The European perspective on nitrogen emission and deposition.

Europe has been successful in reducing the emissions of several nitrogenous pollutants over recent decades. This is reflected in concentrations and deposition rates that have decreased for several components. Emissions of nitrogen containing gases are estimated to have decreased in Europe by 10%, 21% and 14% for N(2)O, NO(x) and NH(3), respectively, between 1990 and 1998. The main reductions are the result of a decrease in industrial and agricultural activities in the east of Europe. The reductions are a result of the economic situation, measures in the transport sector, industry, and the agricultural sector, with only a small part of the reduction due to specific measures designed to reduce emissions. The reduction is significant but far from the end goal for large areas in Europe, in relation to different environmental problems. The Gothenburg Protocol will lead to reductions of 50% and 12% in 2010 relative to 1990 for NO(x) and NH(3), respectively. The N(2)O emissions are expected to grow by 9% between 1998 and 2010. Further reductions are necessary to reach critical limits for ecosystem protection, air quality standards, and climate change. Emissions of nitrogen compounds result from an overload of reactive nitrogen that is produced by combustion processes, by synthesis of ammonia, or by import from other areas as concentrated animal feeds. Some improvements can be made in the efficiency of combustion processes and agricultural systems. However, measures to reduce emissions substantially need to focus on decreasing the production or import of reactive N. Reactive N ceilings for regions, based on critical limits for all N-related effects, can help to focus such measures. An integrated approach might have advantages over the pollutant-specific approach, to combat nitrogen pollution. This could provide the future direction for European policy to reduce the impacts of excess nitrogen.

Deposition to forests in Europe: most important factors influencing dry deposition and models used for generalisation.

Dry deposition of gases and particles to forests is influenced by factors influencing the turbulent transport, such as wind speed, tree height, canopy closure, LAI, etc. as well as by factors influencing surface condition, such as precipitation, relative humidity, global radiation, etc. In this paper, an overview of these factors is given and it is shown which are the most important determining temporal and spatial variation of dry deposition of sodium and sulphur. Furthermore, it is evaluated how well current deposition models are able to describe the temporal and spatial variation in dry deposition. It is concluded that the temporal variation is not modelled well enough, because of limited surface-wetness exchange parameterisations. The influence of forest characteristics are modelled reasonably well, provided enough data describing the forests and the spatial variation in concentration is available. For Europe these data are not available. The means to decrease the atmospheric deposition through forest management is discussed.

Field intercomparison of throughfall measurements performed within the framework of the Pan European intensive monitoring program of EU/ICP Forest.

A 6-month field intercomparison study on throughfall measurements was performed at Speulder forest near the west coast in The Netherlands. Twenty throughfall sampling systems were evaluated on accuracy, sampling strategy and performance under field conditions. Throughfall fluxes of NO3-, K+ and Kjeldahl-N generally could be determined with a larger accuracy than fluxes of SO4(2-), NH4+, Na+, Cl-, Mg2+, Ca2+, and alkalinity. Throughfall fluxes of H+ generally had the lowest accuracy. Only 20% of the sampling systems differed more than 20% from the best estimate, whereas 45% of the systems stayed within a 10% range from the best estimate. The difference from the best estimate was mainly caused by aspects related to sampling strategy, like, for example, collecting area, sampler placement. The inaccuracy induced by the sampling system appeared to be much larger than that resulting from the analysis of the samples by different laboratory as determined by ring-tests. The field intercomparison described in this article gave a good insight in the different aspects contributing to the overall accuracy of the measurements. However, performing a future field intercomparison is recommended for throughfall and stemflow in order to also take in account other aspects that might influence the performance of the different measurement systems (e.g. tree species, climate zone, summer/winter period).