This action might not be possible to undo. Are you sure you want to continue?
Reduced nitrogen in ecology and the environment
J.W. Erisman a,*, A. Bleeker a, J. Galloway b, M.S. Sutton c
b a Energy Research Center of the Netherlands, ECN, P.O. Box 1, 1755 ZG Petten, The Netherlands Environmental Sciences, University of Virginia, P.O. Box 400123, 291 McCormick Road, Charlottesville, VA 22904, USA c CEH, Bush Estate, Penicuik, Midlothian EH26 0QB, UK
Received 11 June 2007; accepted 11 June 2007
Half of industrial ammonia production is eventually lost to the global environment with signiﬁcant effects.
Abstract Since the beginning of the 19th century humans have increasingly ﬁxed atmospheric nitrogen as ammonia to be used as fertilizer. The fertilizers are necessary to create amino acids and carbohydrates in plants to feed animals and humans. The efﬁciency with which the fertilizers eventually reach humans is very small: 5e15%, with much of the remainder lost to the environment. The global industrial production of ammonia amounts to 117 Mton NH3-N yearÀ1 (for 2004). By comparison, we calculate that anthropogenic emissions of NH3 to the atmosphere over the lifecycle of industrial NH3 in agriculture are 45.3 Mton NH3-N yearÀ1, about half the industrial production. Once emitted ammonia has a central role in many environmental issues. We expect an increase in fertilizer use through increasing demands for food and biofuels as population increases. Therefore, management of ammonia or abatement is necessary. Ó 2007 Elsevier Ltd. All rights reserved.
Keywords: Reduced nitrogen; Emission; Nitrogen cycle; Ammonia; Effects; Abatement
1. Introduction In 1827 the German professor Von Liebig (1827) reported that about 27 kg/ha free fertilizer was obtained by wet deposition from the atmosphere, which was regarded as so much that additional fertilizer was not necessary to grow plants. Since that time a debate was started on the validity of this number and the start of fertilizer and environmental ammonia research was a fact. Von Liebig appeared to be wrong at that time, overestimating the atmospheric deposition as a result of measurement errors. However, in large industrialized parts of the world the current deposition far exceeds this number as the result of increased intensities of agriculture, industrial processes and trafﬁc. The central role of ammonia in environmental problems is now becoming more widely recognized.
* Corresponding author. E-mail address: email@example.com (J.W. Erisman). 0269-7491/$ - see front matter Ó 2007 Elsevier Ltd. All rights reserved. doi:10.1016/j.envpol.2007.06.033
Nitrogen, present in amino acids, proteins, and DNA, is necessary for life. While there is an abundance of nitrogen in nature, almost all is in an unreactive form (gaseous nitrogen, N2) that is not usable by most organisms. In the absence of human intervention, the supply of reactive nitrogen in the environment is not sufﬁcient to sustain the current abundance of human life. Thus humans learned in the early 20th century how to convert gaseous N2 into forms that could sustain food production. Over 40% of the world’s population is here today because of that capability. There are two major problems with nitrogen: some regions of the world do not have enough reactive nitrogen to sustain human life, resulting in hunger and malnutrition, while other regions have too much nitrogen (mainly due to the burning of fossil fuel and inefﬁcient incorporation of nitrogen into food products) resulting in a large number of major human health and ecological effects (e.g. Vitousek et al., 1997; Mansﬁeld et al., 1998; Langan, 1999; Erisman et al., 1998a,b; Cowling et al., 2001; Galloway et al., 2003). The rate of
Aquatic systems primarily contain soluble forms of nitrogen. Besides plant use of nitrate. however. RNA. Some of this is captured by photosynthesis. Urea. Since today’s most primitive life forms are anaerobic. Oxygen prevents growth of the most primitive living bacteria such as photosynthetic bacteria. Whereas the (Second) atmosphere was composed of high concentrations of ammonia. Reduced nitrogen. The scientiﬁc basis for reduced nitrogen in ecology and in the environment needs to be strengthened. the current atmosphere has a high oxidizing capacity. The nitrogen cycle Nitrogen is an important element e the most abundant constituent of the atmosphere. Produced O2 levels by breakup of water molecules by ultraviolet were approx. ammonia coexists in both the protonated and de-protonated forms near neutral pH. is essential in food production. Although reduced nitrogen is preferred for biosynthetic reactions.W. and other compounds that make up living systems. such as oxygen. produced by cyanobacteria. is hydrolysed readily in the environment into ammonia and carbon dioxide. methane-producing bacteria. the ﬁrst forms of cellular life probably had similar metabolisms. Living systems are essential for maintaining the balance between nitrogen’s reduced and oxidized forms. We learn from the past that volcanic emissions are an important source for ammonia in the atmosphere. We here summarize the issues associated with increased ammonia emissions and discuss the need and possibilities for abatement measures. The Earth’s surface receives an average radiation input of 100e 300 W/m2/day. Emissions of ammonia to the atmosphere can contribute to particulate matter formation affecting human health. by de-nitriﬁcation processes (the conversion of nitrate to N2 and N2O). such as nitrate and ammonia/ammonium ion. 2. This was an evolutionary necessity because nitrate is the dominant soluble form of nitrogen in aerated soils. Gases produced were probably similar to those created by modern volcanoes (H2O. The amount of O2 in the atmosphere has increased with time. At these levels Ozone (O3) can form to shield Earth’s surface from UV. we speak of the First Atmosphere. Such a cycle is often termed a biogeochemical cycle because chemistry. its .J. allowing oceans to form. ammonium and amines. probably greater than that for any other major ecological problem. depending on latitude. DNA. and lagoons. nitrogen dioxide. Nearly all organisms can use ammonia for biosynthesis (ammonia assimilation). The least known part of the nitrogen cycle is the reduced nitrogen form. These gases are relatively rare on Earth compared to other places in the universe and were probably lost to space early in Earth’s history because Earth’s gravity was not strong enough to hold lighter gases. and RNA). as in the bacterial decomposition of dead organisms (ammoniﬁcation). Ammonia in the early atmosphere Before the Earth’s crust was formed. Cl2. and nitrous oxide). along with other trace gases (ammonia. S2. The ultimate source of energy for driving energetically uphill reactions is the sun. Fig. Erisman et al. 1e2% current levels. NH3 (ammonia) and CH4 (methane). 2. Nowadays the atmosphere contains mostly elemental dinitrogen. CO. The most important aspect of the environmental nitrogen cycle is the dynamic exchange of species that occurs between the atmosphere and the surface landmasses and oceans. contributing to the greenhouse effect. and H2). and bacteria that derive energy from fermentation.1. H2O produced by out gassing could exist as liquid in the Early Archean. Since lone pairs of electrons on nitrogen are usually basic. Today these anaerobic life forms are restricted to anoxic (low oxygen) habitats such as swamps. Once the core differentiated the heavier gases could be retained and the Second Atmosphere was formed mainly by volcanic out gassing. CO2. 1 shows the nitrogen cycle in its most elemental form. biology. Reduced nitrogen has a crucial role in ecology and in the environment. biosynthesis (making amino acids. in ecology and also in the environment. Chemical building blocks of life could not have been formed in the presence of atmospheric oxygen. A prerequisite to reduce these problems is the development of a sound scientiﬁc base on which to begin to discuss policy options. as well as biological nitrogen found in proteins. Today. contributing to eutrophication and acidiﬁcation of aquatic and terrestrial ecosystems after deposition and to nitrous oxide formation. the atmosphere is w21% free oxygen. It is useful to look at the reactions of elements in the form of a closed cycle. N2. comprising probably entirely of H2 and He. Mammals eliminate ammonia. nitric oxide. As the Earth cooled. and used to produce high-energy content molecules. the liver transforms it into the less toxic compound urea before excreting it. and nitrogen ﬁxation (reduction of N2 to NH3 by bacteria in root nodules). Formation of reduced nitrogen compounds is energetically uphill. Cycling of elements is often governed by kinetics and may involve the input of energy. SO2. and geology all provide important inputs. so that chemical equilibrium states are not attained. which accounts for ammonia emissions from animal feedlots. such as ammonia. half of the synthetic nitrogen fertilizer ever used on Earth has been used in just the last 15e20 years. No free O2 existed at this time (not found in volcanic gases). plants have also learnt to capture the nitrogen they need by assimilatory nitrate reduction. / Environmental Pollution 150 (2007) 140e149 141 change of the problem is tremendous. Photosynthesis combined CO2 þ H2O þ sunlight into the formation of organic compounds and O2. Ammonia is also a major metabolic end product. ponds. and eventually higher plants e supplied the rest of O2 to the atmosphere. which is prepared industrially at high pressure from the reaction between ammonia and carbon dioxide. For example. It is also one of the essential elements for the growth of plants and animals. Chemical reactions that yield amino acids are inhibited by the presence of very small amounts of oxygen. DNA. They play an important role in providing reduced nitrogen compounds for the global cycle. Opportunities to reduce these problems are plentiful.
3. for explosives and as a refrigerator replacement for chloroﬂuorocarbons. The average price is about $100/ton NH3. This will drive ammonia prices down towards their historic average of about $150/ton NH3. the ammonia (and fertilizer) price is strongly coupled to the natural gas and thus the oil price. The remainder is used in a wide range of processes. / Environmental Pollution 150 (2007) 140e149 concentrate removed from cycle atmospheric deposition NOy. Annually this yields about 11 billion $. 2001). In addition. . With these reagents it is ultimately possible to synthesize any desired intermediate oxidation state of nitrogen. 2. gradually fertilization became more speciﬁc and adapted to plant needs.W. 1.. which will keep the fertilizer price at low levels. Furthermore. Erisman.. including the production of caprolactam (basis for nylon) and acrylonitril for acryl ﬁbers. reduction also occurs by bacterial action in oxygen-free soil and sediment environments. submitted for publication). Erisman et al.142 J. The Fertilizer Handbook). After the invention and implementation of the HabereBosch process to produce NH3 from N2 and hydrogen. nitric acid. Since it was discovered that ammonia is the key element for plant growth by Von Liebig (1827). Sutton et al. 2 shows the NH3 price since 1970. Human creation of reduced nitrogen If we go back into history. The economic value of NH3 is enormous. 2006). 80% of the chemical production of NH3 is used to produce fertilizer in the forms of ammonium nitrate. Fig. creating and adding them (Smil. Ammonia is oxidized to produce nitric acid in another reaction. such as clover and alfalfa. An investment of $120 per ha has been estimated to yield a net return of $925. called the Oswald process after its discoverer Wilhelm Oswald. the production increased rapidly (Smil. 2006). calcium nitrate. Ammonia is one of the major gaseous products of global chemical industry. both industrially as well as for fertilizers.NHx atmospheric N2 Industrial fixation symbiotic fixation (legumes) nitrogen fertilizer NH3 N2 N2 O crop residu manure soil organic matter plant uptake immobilisation ammonium NH4 nitrate NO3– nitrification ammonification denitrification leaching Fig. in a later stage transporting them from concentrated areas (Guano). ammonium bicarbonate and several varieties NPK (mixtures of nitrogen. The investment for farmers in fertilizer is very proﬁtable. 2001. the main use of which is in fertilizer production for food and ﬁbre production. The second largest bulk industrial nitrogen feedstock. which ﬁxes nitrogen to ammonia on a large scale in the HabereBosch process. urea. The rates of global ammonia manufacture since 1900 are shown in Fig. it is substantial that new ammonia production capacity will come on line in the next 4 years (Gosnell. lies at the other extreme of the redox series. It makes good chemical sense that the principal industrial nitrogen compounds lie at opposite ends of the redox series. Fritz Haber and Carl Bosch developed the ﬁrst high pressure industrial process. man has searched ways for centuries to increase the production of food by conserving the nutrients or. a factor of 7 (Yara. and phosphorus). for the future use of ammonia in combination with fuel cells as an emission-free transportation fuel is suggested as a serious option (Christensen et al. 2000. potassium. For example. The most important elements of the nitrogen cycle. Overall. Because of the high-energy requirements of the HabereBosch process. nitrogen-ﬁxing bacteria create their own oxygen-free environment in aerated soils by forming nodules on the roots of legumes.
The data from different sources in Table 1 reﬂect the variation in estimates. 2. 1999). the emissions might directly or indirectly lead to environmental impacts. The ﬁrst 100 kg/ha of fertilizer N is three times as effective for crop growth as the second hundred (Socolow.9 1. and Battye et al. 2006).7 21. with NH3 emissions from ammonium sulphate being typically 5e15%. with typical NH3 losses after ﬁeld application of 1e2%.3 8. The global NH3 emission is estimated to be 53. 2001). while those from urea are typically 10e20% (EEA. / Environmental Pollution 150 (2007) 140e149 120000 500 143 Global Fertilizer and Industrial NH3 production (1000ton) 100000 Industrial ammonia production Agricultural NH3 emissions Ammonia emissions Fertilizer production N2O emission 450 400 350 80000 US $/ton US$/ton NH3 300 60000 250 200 40000 150 100 50 0 1910 0 1920 1930 1940 1950 1960 1970 1980 1990 2000 20000 year Fig. can be large in areas with intensive livestock breeding. Bouwman et al.2 53. 1997) Source Dairy cattle Non-dairy cattle Buffaloes Pigs Poultry Sheep/goats Other animals Subtotal domestic animals Fertilizers Agricultural crops Biomass burning Seas Other sources Total Ammonia emission (106 ton N yearÀ1) 4. Nevertheless. Erisman (2000). The efﬁciency with which the fertilizers eventually reach humans is therefore very small: 14% for vegetarians and only 4% for omnivores (Smil. 2002).2 3. There are several studies that provide an overview of ammonia emissions to the environment. However. including the amount which is used for fertilizer production (http://minerals. Currently volcanic emissions are not included in the emission inventories and might contribute to the global balance. These emissions are not relevant on a global scale. These emissions.7 Tg N of which 10. which means that within the cascade nitrogen losses will occur (Galloway et al.7 % 8 16 2 6 4 3 1 40 17 7 8 15 13 100 .gov/index.6 4. Ammonia is a key gas in atmospheric chemistry.4 1. however.J. The world average fertilizer use in 2001 was 90 kg/ha of agricultural land. 4. with a strong difference between excess areas and areas where there is shortage. EEA (2002). Direct losses of ammonia during industrial production are relatively small because of the stringent safety regulations and the economic value of ammonia. because the nitrogen use efﬁciency (NUE) is much less than 100%. 2001. Historical US Gulf Coast NH3 Prices (Gosnell..2 (Congo) to 562 kg/ha in Ireland (Earth Trends Data Tables).usgs.0 3.6 1.. (2003).5 0. 1998). airesurface exchange processes and environmental effects. where the optimum nitrogen is exceeded.html) and the NH3 and N2O emissions to the atmosphere since 1900 (Olivier et al. 1998..7 Tg is of natural origin about 65% is from agriculture and 16% is natural (Table 1). the rest is returned to the atmosphere as N2 or lost to the environment. in other areas. environmental losses are unavoidable even where fertilizers with low NH3 emissions are used.2 7..1 8. In nitrogen poor areas crop production might beneﬁt from the ammonia emissions.W. ranging from 0. Emissions of ammonia to the atmosphere It is well-known that ammonia can be emitted into the atmosphere from animal manure and was already demonstrated by Way (1856). such as Buijsman et al. which are an indirect result of the ammonia fertilizer application in the nitrogen cycle.6 9. 2002). Only about 10e30% of the nitrogen is used in end products (Smil. Other natural emissions come from large colonies of seals or penguins. Global industrial production of NH3. (1987). Fertilizers are also optimized for crop production and losses should be minimized when applied in the ﬁeld. but might contribute locally to nitrogen enrichment and Table 1 Global atmospheric sources of ammonia (Asman et al. Erisman et al. The best performance is for ammonium nitrate fertilizer. some fertilizers are less efﬁcient. 2003).
9 Tg N). Pratt (2006) measured high ammonia concentrations in caves. Atmospheric transport and atmosphereebiosphere exchange Recently several papers giving overviews of the atmosphereebiosphere interactions have been published (e.g.org/docrep/W5146E/w5146e00. and relative humidity) and soil properties. This holds for the urban emissions of cars. 2007).. in press). 2003. 2005a. household application of ammonia. The emissions are mainly concentrated in the Northern Hemisphere (e. emissions of amines and ammonia emissions. This leaves the amount of reactive nitrogen that is eventually lost to the environment as the result of fertilizer highly uncertain. (1998).W. There are some environments. industry (Erisman. and are ideal to study the ammonia emissions and transport. Other sources include biomass burning. vegetation. . which has a relevance in human health reduction and plays a role in climate cooling. e. precipitation. The main agricultural sources are also given in Table 1.it forms particulate matter (ammonium nitrate and sulphates).htm# Contents) were taken to translate the trend up to 1995 into data for 2005. / Environmental Pollution 150 (2007) 140e149 because they are isolated hotspots. neutralizing toxic acids. (1998). The relevance for reduced nitrogen in the atmosphere is: . Although these sources only comprise a minor part of the emissions. We are currently able to model the emissions on an annual basis. Fig. This is called the Enigma of the Nitrogen balance by Allison (1955).it provides a means to transport reactive nitrogen to other areas. One might expect that the emission factors increase with higher inputs of nitrogen as fertilizer. Ansari and Pandis. 2 shows that by combining different statistical data from different sources questions can be raised about the inconsistency of the results. Furthermore. Locally. however.. and Bouwman et al. 2006).. submitted for publication). The spatial scale needs to be reﬁned in order to meet the requirements of dispersion models to assess the transport and deposition.mnp. climate (wind.144 J.. 1994). When using emission inventories the temporal variation needs to be addressed separately (Hellsten et al. similar to that estimated for the Eastern part of North Carolina (Cowling et al. This means that the emission factors in the past are either overestimated. cars equipped with a three-way catalyst.b. there is a retention in the emissions related to fertilizer application. where source and sink terms are highly variable in time and space.g. Especially in systems where there is a high protein diet for the animals the emissions are high. A non-linear relationship is expected. Most important sources are animal excreta (21. Asman et al. excretion factors and emission factors. and Eastern and Central parts of the USA has resulted in increased ammonia emissions. 2 shows the trend in global emission estimates based on statistics and emission factors. Within caves the air stream is limited and no dilution takes place. There is still a big gap in the Nitrogen balance at different scales. The data up to 1995 stem from Olivier et al. 1998). Krupa. the ammonium content in manure. The driving forces for emissions of reduced forms of nitrogen are the protein uptake of animals. There is evidence that other . might play a role. Sutton et al. coal burning. 2007. The FAO scenarios on global agricultural activities (http://www. or current emissions are underestimated. when converted into ammonium the atmospheric lifetime could be extended up to 1 week. Fig. 2007).fao. 1998). in the Netherlands the emission is on the average 30 kg/ha. India. Ammonia emissions are based on animal numbers. because the nitrogen use efﬁciency decreases with higher inputs. Even within these areas there is a large variation in the spatial distribution of the emissions. Much farm-level research has shown that the gap between input and output of N can be up to 40% (Oenema et al. The animals and other organisms living in the caves are gradually adapted to the high concentrations (Pratt. and biomass burning (5. However. ¨ During the last 30 years a strong increase in fertilizer use and in livestock breeding in China. even though organic nitrogen. 1) and then cascades through the environment. pets and industries. Animal husbandry is the most important source. Erisman et al. South Korea. The data suggest that until 1965 ammonia emissions were higher than the industrial ammonia production and the ratio reduced to almost 50% in 2005. Bleeker et al. but with a gradual increase because of intensiﬁcation and decreasing efﬁciency. and . The emissions result from housing systems and application of manure in the ﬁeld. This reﬂects the uncertainty in the ammonia emissions. in press). It demonstrates that the ammonia emissions are uncertain and there is a need to estimate the emissions as the result of a Nitrogen balance model (Dammgen and Hutchings. the temporal variation in emission factors can be very large both from day to day as well as during the seasons. housing systems.. In some caves bats’ droppings emit ammonia and also goats’ and/or sheep dung emits ammonia and measured concentrations range from 2 to 2000 ppm (Pratt. because the reactive nitrogen ﬁrst takes part in the cascade on farm-level (see Fig. the emission of ammonia can be much higher. 5.6 Tg N).g. pets. (1997) (see also http://www. It is suspected that denitriﬁcation is the most important process that can explain the gap.g.it provides the only atmospheric base. 2006). Dentener and Crutzen. but also the uncertainty in the cascade of nitrogen that starts with the fertilizer application.nl/edgar/model/ v32ft2000edgar/). The agricultural ammonia emission becomes a smaller part of the fertilizer use in time. Reduced nitrogen is very reactive in the different environments and therefore its lifetime is limited.. 2000). Furthermore. they might be relevant locally. submitted for publication. fertilizer use (9 Tg N). affecting the local chemical climate and forming ammonium aerosols (e. Here only the most important issues are discussed. provided the agricultural data are available (Dammgen and ¨ Hutchings. that make that ammonia can exist. Inventories of agricultural emissions are becoming available for different areas of Europe and North America. The emission factors are constant in time and the linear relation between animal numbers therefore determines the trend in ammonia emissions. Erisman et al.
1998a.. Furthermore. Originally the ammonia gap existed in two parts: (i) an absolute difference between measurements and concentrations based on modelling. The EMEP monitoring sites that have been in place are not aimed to detect ammonia from agriculture and therefore the signal is not detectable.. Short-term changes in emissions are not well quantiﬁed. 2005). in order to effectively detect the expected emission changes within different regions.e. / Environmental Pollution 150 (2007) 140e149 145 animals and even humans will not expose themselves to these concentrations. nor in the emissions. Bleeker et al.. where emissions decreased by about 30%. Another case in the UK. There are differences in aerosol neutralization in Europe and North America leading to different appreciations of the role of NH3 in atmospheric chemistry. For the whole of Europe it is questionable if the decrease in emissions that took place in the early nineties as the result of the poor economics in the Eastern part of Europe can be detected. Uncertainty in the size and sign of the spatial distribution of the airesea ﬂux of ammonia is mainly due to the poorly deﬁned concentration driving force (difference between normalized air and water concentrations). making an explanation for the so-called ‘ammonia gap’ possible (Erisman et al. models and monitoring equipment) to evaluate the link between ammonia emission and the concentration and/or deposition of reduced nitrogen has improved. The uncertainty in these models is dominated by the cuticle (and water layer) uptake and release of ammonia and the apoplast concentrations regulating the exchange between the atmosphere and stomata (Nemitz et al. Clear trends from this network could not be found. This is especially true for the situation in Denmark and the Netherlands. Apart from the Netherlands and Denmark. nor in the responses in concentrations and deposition. The neutralization factor of aerosol and precipitation might be a good indicator for the relevance and emissions of NH3. 2007). In North America aerosol is generally not neutralized. in North America and in Europe. The role of cuticular resistances in NH3 ﬂuxes to semi-natural vegetation has been shown to be the most important in regulating the deposition ﬂux (Sutton et al. There have been several studies done focussing on explaining these two gaps (see Bleeker et al. Interactions between SO2. 1998. Dry deposition of NH3 close to major sources contributes typically 4e10% of the total emissions within 500 m of the source. 2004). In these countries the emission reductions were only very limited. The explanation of the difference can be by two factors. for the new EMEP monitoring strategy there is lack of implementation especially in Eastern Europe.. The extended data sets made it clear that following emission trends by means of measurements can only adequately be done when long-term measurements are available.. but this is mainly due to only small changes in emission levels. 2007). in most countries where monitoring takes place the concentrations did not change much (UK and Switzerland). based on extensive pre-studies used for developing the measuring networks. There are few reliable measurements. Within the quantiﬁcation of the atmosphereebiosphere interactions of ammonia models have been developed these past years. The long-term measurements for reduced nitrogen follow the emission trend. and Switzerland). It is therefore concluded that the evaluation of the absolute emissions in Europe and the changes therein is difﬁcult because of lack of monitoring data covering the whole of Europe.. Models and input data are still inadequate to show these changes. (2007) provide next to country-speciﬁc case studies. probably contributing both: (i) underestimation of certain emissions. This resistance determines which NH3 concentration and which responses have key implications and more work is necessary. Where substantial reductions have been made the beneﬁts are clear at the decreased scale in aerosol and precipitation composition. improving the emission estimates and taking the meteorological conditions into account this is solved (Van Jaarsveld et al. where it was possible to detect changing emissions in measured concentrations of NH3. This situation is in urgent need of . However. There is no difference between the measured and modelled trend. 2000). inﬂuencing the transport distance of ammonium. also an overview of the European situation with respect to the link between emissions of NH3 and the modelled and measured concentration/deposition of reduced nitrogen. was related to a study following an event of Foot and Mouth Disease in different regions in the UK (Sutton et al. NOX and NHX have created a change in the main form of NHX from (NH4)2SO4 to NH4NO3. Erisman and Monteny. Current measurements make it possible to evaluate policy progress on ammonia emission abatement. submitted for publication. where the NH3 ammonia reduction is followed by the monitoring results from the national monitoring networks. Previous concept of the oceans everywhere being a source of ammonia to the atmosphere is probably wrong. Increases in ambient NH3 and NH4 in ppt in remote areas of Europe require quantitative explanation and more detailed measurements to demonstrate the cause (Fowler et al.. By extending the monitoring period. However. This is troubled by the fact that at the same time the SO2 emissions strongly decreased affecting the lifetime and transport distance of ammonia. Denmark. no systematic gap such as in the Netherlands is signalled (UK. In Europe sulphate is mostly neutralized by ammonia and nitrate equilibrium changes. The UK also performed such a pre-study for developing their national monitoring network. Measurements have shown that low latitude (warm) waters can be regarded as sources.W.. However. This is explained by strong temperature dependence of the Henry’s Law constant for ammonia and leads to a signiﬁcant reduction in the global marine ﬂux of ammonia to the atmosphere. whereas high latitude (cold) waters as sinks. Van Jaarsveld et al. the absolute systematic difference is still in the order of 30%. Responses in ambient concentration and deposition to change in NH3 emission are seasonally well understood. In previous years the instrumentation (i. and (ii) parameterisation (overestimating) of the dry deposition in agricultural areas. and (ii) a difference in trend between measurements and modelled data. Also here a modelling pre-study was used for designing the layout of the measurement network.J. this is only possible since both these networks were designed to follow the expected changes in emissions. 2000). Erisman et al.b. 2000).
One ammonia molecule does not cause one speciﬁc effect. Italy. More recently data have become available showing that reduced nitrogen inputs are more effective in decreasing biodiversity than is oxidized nitrogen (Haddad et al. (1998).W.4 0. 2000 Bobbink. Methylamines are stronger bases than ammonia and so. they can constitute 10e20% of the atmospheric basicity in offshore marine environments.. in press).g.. 2005a. Furthermore. which also contribute to the cooling through the (in)direct aerosol effect (Liao et al. increased levels of ammonium can be toxic to plants (e.. Paulissen et al.. 3... 2000). Pitcairn et al. NH4 is relevant in the exposure of humans through its contribution to particulate matter concentrations (e.g. During the process of nitriﬁcation NO and N2O can be formed. Data sources: Dise and Stevens (2005). 1998.. 6. little research on methylamines and it is advised to foster more research in this area. 2004). The fertilization of the system with ammonia leads to changes in the carbon sequestration affecting climate change (e. Van Breemen et al... (2004). Direct exposure of humans or vegetation to high levels of NH3 can lead to toxiﬁcation and serious effects. Goulding et al. Very high exposure of atmospheric NH3 can be dealt with by the plant until toxicity is reached..8 y = -0. 1998. 2006).g. (2000). 2003. 1999). 2004 Log.8 1.6 groundwater pollution.g. 2004 Haddad et al.... Ansari and Pandis.6 0. but can lead to a cascade of effects (Galloway et al. De Vries et al. NEGTAP. 2004. Finally.37 q 0. Ammonia deposition has a direct relation to eutrophication of surface waters and natural areas. 2003. Aneja et al. however. Erisman et al. 2004.146 J.g. in press). Bobbink. 2004) and illustrated in Fig.4 1. / Environmental Pollution 150 (2007) 140e149 attention if we are to understand the role that ammonia from the oceans plays in particle formation and in controlling the pH of rain and particles in the remote marine atmosphere. 2001). Castro et al. Sub-arctic vegetation is very sensitive to a high nitrogen load. Reduced nitrogen is more readily available. Biodiversity decreases when nitrogen increases as has been shown in the literature (e... Van Grinsven et al. (1982) showed how atmospheric ammonia deposition contributes to soil acidiﬁcation in natural areas where the deposition was up to 120 kg N/ha.2 Ln(x) + 1. although their ﬂuxes across the airesea interface are only a few percent of those for ammonia. Shown is the ratio of the number of species at increased levels compared to those at low level N. Furthermore. Reduced N is much more harmful for (semi)natural vegetation Stevens et al. It has been demonstrated in the lab that plants can grow solemnly on atmospheric NH3.. 2005. Stevens et al.b). Goulding et al.g. .g. Erisman. Stevens et al. Mosier et al. 3. 2007. South Korea.2 1 0. during the last 30 years a strong increase in fertilizer use and in livestock breeding in China. threatening biodiversity (Phoenix et al. submitted for publication). Erisman et al.4 R2 = 0. Root uptake of NO3 is lowered during these exposures. 2001) and the N2O emissions contributing to climate change (e. The ‘burning’ of vegetation has been observed near to intensive livestock breeding farms (e. 2006). India. The combination of acidiﬁcation and eutrophication leads to base cation leaching from the soil and an imbalance in nutrient status (N-excess. Klimek et al. There is. eutrophication of coastal waters and resulting hypoxia (e.g. and Haddad et al. and Eastern and Central parts of the USA has resulted in increased emissions.. the effects of NH3 emissions are less well recognized and often relegated to consideration as a ‘‘local problem’’ in highly intensive livestock breeding areas such as the Netherlands. 2006). deposition of NH3 and NHþ particles can lead to acidiﬁcation damaging 4 the cultural heritage and can contribute to reduced visibility at scenic vistas and airports.. soil acidiﬁcation occurs and nitrate is leached leading to 2 1. Rabalais and Turner. 1998). Number of species in terrestrial systems decreasing with increasing nitrogen input (kg/ha).2 0 0 50 100 150 200 250 300 Total N input Fig. Effects Even though the environmental consequences of fertilizers are well recognized when it comes to nitrate pollution in groundwater (e. Dise and Stevens. There are no indications of toxicity at long-term exposure with low to moderate concentrations of NH3 (Castro et al. (Log function) Number of species ratio 1. However. through nitriﬁcation in the soil. parts of Germany and Denmark. stimulating growth. Bobbink (2004).. 2000. Nadelhoffer et al.
W. doi:10. Smeulders. van der Hoek. Asman. Biomass will have a large contribution to the world energy production. organized in the Universitatszentrum Obergurgl.ac. S.09.html> Bobbink. 2006. Conclusions Currently the ammonia wasted to the atmosphere is about half of the global industrial production of ammonia... Castro.2007. There are also observations of severe effects of reduced N on vascular plants and lichens in the Mediterranean region. 1987. Fowler. V.. Z.H.. V. Christensen. .. T. which has been the case these past years in Europe and USA.A. About 70% of the targets of 20% greenhouse gas emission reduction and a 20% share of sustainable energy in 2020 in Europe will be from biomass. Effects of ammonia to the environment are clearly visible and widespread... De Kok. after saturation of the bog with N. Erisman. pp. improving data on ﬂuxes. J. 213e250. The agricultural area used for food production is not expected to increase to a large degree. Johannessen. Ammonia has therefore become a continental issue. Maas. Optimizing nitrogen management 7. T. D. changing to more productive crops and by increased application of fertilizers. I.. all emphasize the need for more complete scientiﬁc understanding of both the beneﬁcial and detrimental effects and the intended and unintended consequences of continuously increasing circulation of ammonia in commerce and in the atmosphere and the biosphere of the Earth. 2005)..P. 1998.. 1998. Because of the cascade of reduced nitrogen through the agricultural system and the environment an integral approach is needed. However... L.ammoniaws. The enigma of soil nitrogen balance sheets.envpol.. New Phytologist 139. A. Wang. Advances in Agronomy 7. Asman. Smeulders. B. There is a need for a new thorough updating of the N cycle of at least the anthropogenic part..A.. Atmospheric Environment 21. Pandis.021.B. J. Aneja. Haeuber.. Gauger. Kimball. Bouwman. <http://www.N. H.H. Environmental Pollution. Mosier.A..esf.. Sørensen.. Tang.S. Nicholson. Melillo.. Ansari... This is caused by the change in the ratio of SO2 and NH3 emissions. Cowling. S. Fagerli. Ellermann. L. Alebic-Juretic. These effects. H. K. Journal of the Air and Waste Management Association 56..J. this does not imply that oxidized N is less important. 1009e1022.. H.M.P.b).. Asman. Lee.P..S. A global high-resolution emission inventory for ammonia. not only in abiotic heath lands. K.J.. C.H.S. K. NH3 emission increased or remained fairly constant and SO2 decreased affecting aerosol formation and gas deposition inducing important non-linearity’s in sulfur and oxidized nitrogen emissionedeposition relationships and changing deposition patterns (Fowler et al.. Smith. J. Linking Ammonia Emission Trends to Measured Concentrations and Deposition of Reduced Nitrogen at Different Scales.. Bresser. focussed on the reduction of reactive nitrogen formation and/or on the reduction of concentrating nitrogen in intensive agricultural areas.J. Because of the strong link between food production and NH3 emissions.. R.. and uncertainties associated with these effects.. J.. Howarth.. Furthermore... 2005a. Dentener. The estimates of global. Furiness. atmospheric transport and deposition.M. Optimizing air quality management in Europe and North America: justiﬁcation for integrated management of both oxidized and reduced forms of nitrogen. submitted for publication). 561e587. W.. D. Sutton.. in contrast to the world population which will increase for the next few decades. climate and environmental conditions. Moomaw. Cowling. regional and local ammonia emissions have high uncertainties which increase with the smaller scale. W. Aneja. Aneja... Erisman et al.K. ´ Harlen. Atmospheric Environment 37. Acknowledgement This paper is a summary of the most important conclusions of the ESF-FWF Conference in Partnership with LFUI on Reduced Nitrogen in Ecology and the Environment.org/conferences/lc06203). 2706e2714. 10% of the biofuels in the EU and in the US will have to be of biological origin. 1099e1107..Z.F. Nørskov.W. F. van Pul. Utrecht. Bleeker.W.S.. Sutton. Emission factors depend on the type of source. Zhu. 2003. E. We also acknowledge the support of the COST Action 729. J.. J. J. 2001. A.. 2007. reservoirs and also on uncertainties. Battye. Q.. R..1016/j.A. 2004.W.. Y. Plant species richness and the exceedance of empirical nitrogen critical loads: an inventory.. Tong. 1955. the International Nitrogen Initiative (INI) and ESF program Nitrogen in Europe (NinE). Stulen.. S. Bog species are during relatively short-term exposure much more sensitive to NH3 compared to NH4..R. A.J.G. Hole.E..C.. V. T. Holman..I. Towards an ammonia-mediated hydrogen economy? Catalysis Today 111.K. 1997.A. R. 1998.. Acherman. Steger. fens and coastal waters (De Vries et al. it is expected that NH3 emissions will increase in coming years in several areas of the world... 3873e3883. T. E. A. Seitzinger.. Environmental Science and Technology 32. Erisman. J. D..A. E.W. R.. Ammonia: emission. P. Sanders. which needs international agreements on abatement. Utrecht University/RIVM. R. Olivier.. The emission factors probably changed over time because of increased nitrogen fertilization rates. which has not led to a similar decrease in deposition of sulfur in remote (sensitive) areas of Europe. In order to enhance the necessary food and biomass production the productivity of land must increase by intensifying production.W. S.. and the per-capita resource consumption which will increase for decades to come requiring more food and energy (including biomass). M. M. Galloway. B.F.. 27e48.. References Allison.. K..M. Buijsman. Environmental Pollution S1. Atmospheric NH3 as plant nutrient. West. L.. Roelle. C. Another reason for an increasing concern is the successful policy to reduce sulfur emissions... A. J. Austria in 14e18 October ¨ 2006 (http://www. M. Socolow. Global Biogeochemical Cycles 11. Cassman.. 1e19. Mitosinkova. Response of inorganic PM to precursor concentrations. R... 2006. It is known that harmful effect of NH4 occurs after long-term exposure. Walters. W. because further in the cascade the original form of reactive nitrogen is not important (Erisman et al.. F. B. A. Characterization of major chemical components of ﬁne particulate matter in North Carolina. M. Anthropogenic NH3 emissions in Europe. A. and farmer management. Erisman. in press. S. 140e144.H. Horvath. Barber. Background Document.uk/documents. 599e608. Report Landscape Ecology. F.ceh. / Environmental Pollution 150 (2007) 140e149 147 compared to oxidized N. W. grasslands and soft-water lakes but also in ecosystems which are not sensitive to acidiﬁcation like mires. Available from:.. Schjoerring. Evaluation and improvement of ammonia emission inventories.. This should be done for regions and globally.
. Flechard. K. (Eds.W.W.W..W. Erisman. Neftel. M. Erisman.). J. van Grinsven. Olivier. Poulton. History of ammonia. Journal of Geophysical Research D: Atmospheres 109 (16).. 1999. Differential effects of nitrate and ammonium on three fen bryophyte species in relation to pollutant nitrogen input. H.H.S. P.. Bailey.. P.J. 2004. Closing the global N2O budget: nitrous oxide emissions through the agricultural nitrogen cycle: OECD/IPCC/IEA phase II development of IPCC guidelines for national greenhouse gas inventory methodology.148 J.W. 1994. Bouwman. Environmental Pollution 126 (3).A. 2003. 1). Oenema. Erisman. 353e361. Mosquera.. C. van der Hoek.J. Tang. T... Smil. Nitrogen deposition and its contribution to nitrogen cycling and associated soil processes. S. et al....V. Environmental Pollution. E. O. Dordrecht. K. Earth Trends Data Tables. Hargreaves...G... Sutton. 2006.J. Hofmann.J. Y. 14e18 October.. Wageningen. A.J.. 470e476. Di Marco.. J. W. Cowling. S.A.N.. Hellsten. Whitehead. 2002.L.M.. B. Place. Witzke. Global air emission inventories for anthropogenic sources of NOX.017. Nitrogen deposition makes a minor contribution to carbon sequestration in temperate forests. Nadelhoffer.J.T. Van Der Ven. NEGTAP. Gowing. 49e58. J. 2007. T. Skiba... 2005. 2003. Oenema.. U. Soussana. Monteny. 126e131.W. NH3 and N2O in 1990. Herrmann.. (Ghost in a Bottle: Ammonia from Agriculture and the Consequences for the Environment). A.. Nitrogen and food production: proteins for human diets.J.. Y... K. Fowler. vol. J. Effects of atmospheric ammonia (NH3) on terrestrial vegetation: a review.. F..P. S.. L.... Consequences of new scientiﬁc ﬁndings for future abatement of ammonia emissions. J...wri. Erisman. 827e842. Evaluation of ammonia emission abatement on the basis of measurements and model calculations. Kroeze. Bantock. Wisniewski. J. Famulari. Brydges. 73e84.J.E. C. Adverse impacts of increased nitrogen use on terrestrial and aquatic ecosystems. Available from: <http://www. Available from: <http://earthtrends. Hargreaves. T. Oudendag. KBR. S.. 269e274. New Phytologist 139 (1).. Erisman. D. 135e148.W. 2005b.. Crutzen.1016/j. 411 pp.W. 2006. Bioindicators of enhanced nitrogen deposition.J. N.. Cowling. Kluwer Academic Publishers.. J. Environmental Pollution 102..J. C. Science in China 48. Erisman... Leith. third ed.. R. Journal of Atmospheric Chemistry 19. J. Environmental Pollution 102. Sutton. 451e458. Deposition monitoring networks: what monitoring is required to give reasonable estimates of ammonia/ammonium? Environmental Pollution 135. Cosby. Paulissen.D.... de Vries. R. Sheppard. Oecologia 124. N. Velthof.F. Fowler.M.. E. J. Carl Bosch and the Transformation of World Food Production. U. Sutton. 2000.. Murphy. Grennfelt. 271 pp.. J.B....uk/negtap/home.. Vieno.. Horvath. Smil. Butterbach Bahl.. J. 2006.. Satake.F. W. Nordberg. M. (Ed.. Seinfeld. American Geophysical Union.. T.. M. D. Nevison..A. A.ac. O.. Environmental Pollution. N. Kros. N2O and CH4 measurements following the 2001 outbreak of Foot and Mouth Disease in Great Britain to reduce the uncertainties in agricultural emissions abatement. submitted for publication. E... P. Wilson. Enriching the Earth: Fritz Haber. Final Report of the National Expert Group on Transboundary Air Pollution. P. D.F.. Haarstad. Dise.R. M. P. Koopmans. Science in China Series C. B. Gallagher.. C.. Howarth. J. Kros.. R. Dentener. C. J. Dammgen. Sheppard. Dentener. Van Dijk. M. Williams. Kennedy. Van Cleemput. Okello. Wisniewski. R.. the confer-N-s. Cellier... M.J. P.... Global Change Biology 12.. J.J. Berdowski. air quality. P..A.W. de Vries. T.K.L. 1e33. C. Modelling and assessing the spatial distribution of ammonia emissions in the UK. A. Washington..A. Schneider. J.C. New Phytologist 164 (3).. Beier. ISBN 026219449X. Mosier. J.. Erisman. Nitrogen management and the future of food: lessons from the management of energy and carbon. Sanders. 2005a..P. Atmospheric nitrogen deposition in world biodiversity hotspots: the need for a greater global perspective in assessing N deposition impacts. Simmons. G.C.. Pinto. N. Daemmgen.. Draft Final Report (070501/2005/422822/MAR/C1).S. Stevens. Pitcairn.... Mickley.html> Nemitz. Cotrufo.. 2006.A.. Nutrient Cycling in Agroecosystems 52 (2e3). L. Hensen.nbu. Tang... C.. The Dutch N-cascade in the European perspective. H.J.O.J. Phoenix. K.iastate. M. Environmental Pollution 124. ISBN 90-75541-06-6. R. S. D. in food and energy production and environmental protectionProceedings of the Second International Nitrogen Conference on Science and Policy. Fowler... The Scientiﬁc World 1 (S2). G.J. Schjoerring.A. Coastal hypoxia: consequences for living resources and ecosystems... D. N. Austria.. W. de Haan. 2007. V.. 1876e1879. A.J.. Impact of nitrogen deposition on the species richness of grasslands.I.. D. Environmental Pollution 102.. Gosnell.. Schwaiger. 1999. Bull. Plant species richness and composition in managed grasslands: the relative importance of ﬁeld management and environmental factors.03.energy. Erisman.B.K. 2004. Presentation at the ESF-FWF Conference in Partnership with LFUI on Reduced Nitrogen in Ecology and the Environment.. Alterra.. Tietema. Howe. J... 341e356. M.A. 2004.W.. C. submitted for publication.J. Seitzinger. Calanca. 559e570.K.. Bleeker. Emmett. J. O. Brown. Dees.. B. P.. Mansﬁeld. The effects of long-term nitrogen loading on grassland insect communities. C. F. 1998.H. Energy and Chemicals. J.pdf> Haddad. J. P. M. MIT Press. U. van Jaarsveld. S.. I. K.. T. Erisman. Biological Conservation 134 (4).W. Twigg. Socolow.. Dise. N. Science 303 (5665). BetaText.. 1998.... S. U. Nitrogen deposition and reduction of terrestrial biodiversity: evidence from temperate grasslands. 2005.. 145e148.. Goulding. Goulding. 419e431. Proceedings of the National Academy of Sciences of the United States of America 96. M.. 3e12. J.. D. Erisman et al.... Tilman. Loubet.. J. (Eds.V. Environmental Pollution 102 (Suppl. Dragosits. Summary StatementFirst International Nitrogen Conference. U. 405e425. A. Sutton. De Vries. / Environmental Pollution 150 (2007) 140e149 Liao. Gundersen.. Langan. A. L.. Smith. J. in press. N..envpol. .. V.P. 1998. 1998. Smeulders. Nemitz. Isselstein..W. The nitrogen cascade.. J. Life Sciences/Chinese Academy of Sciences 48. 275e282. E. 331e369. Misselbrook. M.. Joint EMEP/CORINAIR Atmospheric Emission Inventory Guidebook. K. S.). Sutton. G. J. Global radiative forcing of coupled tropospheric ozone and aerosols in a uniﬁed general circulation model. Erisman. climate and human health in Europe: an overview. G. Cape.W. Sutton... 2004... N.J. Skiba. 2001. Emissions of gaseous nitrogen species from ¨ manure management e a new approach. B. Agricultural and Forest Meteorology 105.. K. Environmental Pollution..J. D.. Monteny.. 6001e6008. 2001. A. Muller.W.. U. Stevens. K. Britz. L. Galloway.W.. Rabalais. Hutchings. J. Environmental Pollution. J. K.N. O.. Available from: <http://www. The potential of NH3..E. Erisman. S. J.B. J. Pratt. M. M. N.. Environmental Science and Policy 7. Bergen. G. M.P. the Netherlands.D. J. 179e221.R. Fowler.. 2003. Sutton.J.org/datatables/index. Adams. Efﬁcient Ammonia Production. Kjønaas.J. Hobbs..... E.M.W. F.... 1998. 2002. European Environment Agency. P. V. J. Turner. 1998. Klimek.N.R. J. Coastal and Estuarine Studies 58. Nitrogen.T. W. E.P.. European Environment Agency. Krupa. Schjoerring.. Husted.edu/becon/download%20NH3/2005/Gosnell_production. M. (In Dutch).J. J. Laville.R. Kemmermann gen.W..M... Sutton. Resistance modelling of ammonia exchange over oilseed rape. Cambridge University Press. L. Service Contract: Integrated Measures in Agriculture to Reduce Ammonia Emissions.. doi:10. de Vries. 1999.. submitted for publication.A. J. 2000.. Aber.J. the Netherlands.. D. Wright. Bioscience 53.. 177e194... Dragosits.. 2001. Nature 398.J. 225e248. 2000. B. Seitzinger.. 1e9... P. P. Bradbury.. 1998a. Copenhagen.W.php?theme¼8> Erisman. A.. A three-dimensional model of the global ammonia cycle. A.R. Mountford. J.J. B. Wyers. L. C. R. Ambio 31. 139.G. Schleppi. Bobbink. Universitats¨ zentrum Obergurgl. Dore. Jones. Y. 720e728. D. 41e46.).W. Van der Hoek. New Phytologist. the Netherlands. De vliegende geest: ammoniak uit de landbouw en de gevolgen voor de natuur.. Ambio 34 (1). Major Biological Issues Resulting from Anthropogenic Disturbance of the Nitrogen Cycle. Pietrzak. K. McDonald. W. I..... Domburg.2007... The Impact of Nitrogen Deposition on Natural and Semi-natural Ecosystems. Nonlinearities in source receptor relationships for sulfur and nitrogen compounds.
Journal of the Royal Agricultural Society of England 17. Smith. P.. Milne.. RIVM Report No. N. Brueggemann. T. Annales de Chimie et de Physique 35.. Available from: <http://www. J. J.E. Levy.D.F.. E.W.W. M.. Yara. M. Aber.W..W.. N. Burrough. 1997. G... B. Kesik.. 2000. Hoogervorst. 2006... Tilman.. Bergamaschi.com/en/in vestor_relations/presentations/fertilizer_handbook/index.A. J. P. 1827.. C. J. Pilegaard.J. D. 737e750. H.. Ridder..H. Reis. T. Campbell.G. Dragosits.H. K.A. 548e550. de Kok. T. Ecological Applications 7 (3). Schlesinger. U. Reinders. van Dobben.. Vuichard... J. Evaluation of Ammonia Reduction by Means of Measurements and Model Calculations.C... T. D. H.. Velthorst.M. R. Tietema. 125e139. National Institute of Public Health and Environment. Van Grinsven. Challenges in quantifying biosphereeatmosphere exchange of nitrogen species. Human alteration of the global nitrogen cycle: sources and consequences. W. 1982. Sur la nitriﬁcation. Does the evidence about health risks associated with nitrate ingestion warrant an increase of the nitrate standard for drinking water? Environmental Health: A Global Access Science Source 5. Way.. Olesen. N... 149 Van Jaarsveld.U.. R. A. P. 722108025. 2007.J. S.. Matson. Vesala. N.M..B. Vitousek. D.R. Soil acidiﬁcation from atmospheric ammonium sulphate in forest canopy throughfall.. Theobald. Howarth.R. 26.J. 123e162.P.. The Fertilizer Handbook. Bleeker. Nature 299. Environmental Pollution 150 (1).html> . de Wit. Mobbs. Likens.. N. 1856.. Erisman et al. On the composition of land-drainage and of rain. P.. Fowler.. Smith.. Van Breemen. H. the Netherlands (in Dutch).. Ward.L. / Environmental Pollution 150 (2007) 140e149 Emmett..P.A... Pe~nuelas....A.yara. N.F..J.. J. Benjamin. A. J.E. 329. M. D. Von Liebig. Schindler. P.T. Viovy.. J.
This action might not be possible to undo. Are you sure you want to continue?
We've moved you to where you read on your other device.
Get the full title to continue reading from where you left off, or restart the preview.