anthropogenic nh3 emissions in europe

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Jun 15, 1986 - ture. J. envir. Qual. 3, 258-261. Ball R. D., Keeney D. R., Theobald P. W. and Nes P. (1979) .... Hessisches Statistisches Landesamt (1983) Viehbestiinde am 3. Dezember 1982 in den ... Agr. 35, 1297-1310. Sanders L. ( 1980) ...
Atmospheric Environment Vol. 21, No. 5, pp. 1009-1022, 1987. Printed in Great Britain.

0004-6981/87 $3.00+0.00

© 1987 Pergamon Journals Ltd.

ANTHROPOGENIC NH 3 EMISSIONS IN EUROPE Eo BuusMAN*, HANS F. M. MAAS and

WILLEM

A. H. AsMAN

Institute for Meteorology and Oceanography, State University Utrecht, 5 Princetonplein, 3584 CC Utrecht, The Netherlands

(First received 15 June 1986 and received for publication 9 October 1986) Abstract-The first ammonia emission survey with spatially detailed information is presented. Sources of atmospheric ammonia considered include livestock wastes, fertilizers and some industrial activities. The countries involved are 26 European and 1 Asian country. The total ammonia emission is approximately 6.4 Mt of NH 3 a- 1 with a major contribution (81 %) from livestock wastes. Calculations, showing spatially detailed emission data, are made for the grid elements of the EMEP grid (150 x 150 km 2 at 60° N). Emissions in grid elements range from 200 to 4000 kg NH 3 km - 2 a-t.

Key word index: NH 3 , inventory. INTRODUCfiON

Until now much attention has been paid to the significance of atmospheric S0 2 and NOx and their reaction products, especially in relation to the acid rain problem and the long range transport of air pollutants. Much less research has been done on atmospheric ammonia, although it is well known that over large areas in Europe acid precipitation is falling in which up to 70% of the original acid is neutralized by NH3 (EMEP/CCC, 1984). Furthermore in some places serious acidifying effects have been observed which could be attributed to wet deposition of ammonium and dry deposition of NH 3 and ammonium aerosol (Van Breemen et al., 1982). Van Breemen et al. (1982) suggest that nitrification in the soil occurs by Nitrosomas and Nitrobacter bacteria according to the overall reaction: NHt

+ 20 2 -+ 2H + + N03 + H20.

Also NH 3 is an important substance in cloud and rainwater chemistry. Due to its basic character it influences the oxidation rate of dissolved S02 which is higher at higher pH-values (Junge and Ryan, 1958; Adewuyi and Carmichael, 1982; Maahs, 1983). In order to assess the role of atmospheric NH 3 it is important to obtain quantitative information about emissions, atmospheric concentrations, atmospheric transformation rates, transport and the wet and dry deposition flux. In view of the modelling of the long range transport of NH 3 it is important to know as precisely as possible the magnitude and the geographical distribution of NH3 sources. The aim of this paper is to describe a NH3 emission inventory for Europe based on the ~MEP-grid system (EMEP/CCC, 1980). The emission lflventory includes 27 countries: 26 European coun-

tries, of which of the U.S.S.R. only the W part is considered, plus Turkey. By doing so we covered almost the same area as is done for the EMEP S0 2 and NOx emission inventories (Semb and Amble, 1981; EMEP/CCC, 1980). To facilitate the use of the NH 3 emission survey for the evaluation of the impact of decisions in environmental policy, emissions for different source categories are calculated for each grid element. Calculations for a grid system with smaller elements (approximately 75 x 75 km 2) have also been made. Results referring to this grid system (lE-grid) are not discussed here. Details can ·be found in Buijsman et al. (1985). SOURCES OF ATMOSPHERIC NH 3

Important sources of atmospheric NH 3 are considered to be: animal wastes, fertilizers and some industrial activities (Bottger et al., 1978; Bonis et al., 1980; Soderlund and Svensson, 1976; Cass et al., 1982). Sources of minor importance include: traffic (Harkins and Nicksic, 1967; Bonis et al., 1980), natural soils (Bottger et al., 1978), coal combustion (Freyer, 1978), cats and dogs (Cass et al., 1982), human respiration (Larson et al., 1977), sewage sludge (King, 1973; Beauchamp et al., 1978) and wild animals (Soderlund and Svensson, 1976). A detailed overview of NH 3sources has been published by the National Research Council (1978). Global emission surveys have been presented by Robinson and Robbins (1970), Soderlund and Svensson (1976), Bottger et al. (1978) and Meszaros (1981). European emissions were calculated by Bonis et al. (1980), while Soderlund (1977) considered the NW part of Europe. Emission surveys for smaller areas, but with detailed information about the geographical distribution of the sources, were published by Cass et al., (1982) for California, U.S.A., and by Buijsman et al. (1984) for the Netherlands. Although most authors opinions about the absolute

*Present address: RIVM, P.O. Box 1, 3720 BA Bilthoven, The Netherlands. 1009

Eo BuusMAN et al.

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values of the emissions differ, they all consider animal wastes and fertilizers to be responsible for 90% or more of the anthropogenic NH 3 emission. Therefore we have focussed our main attention on these sources.

NH 3 -EMISSION FROM ANIMAL WASTES

Livestock statistics Livestock statistics were primarily taken from publications of national statistical or agricultural organizations. Otherwise information was taken from FAO (1982a). For all countries involved at least the following animal types were taken into account: cattle, pigs, horses, sheep and poultry. In some countries other animals appeared to be quantitatively important (goats, mules, asses or camels), then these animal types were included as well. The amount of waste produced by animals is dependent on age (or weight); as a consequence the NH 3 emission is age (or weight) dependent. Thus, we used information about the age or weight distribution within an animal category. When such information in a country for a certain animal category was not available we assumed a standard distribution as given by CEC (1978b). An overview of

the total number of different animals is given in Table 1. Sources from which the information was obtained are given in Appendix I. In view of our aim to calculate emissions in grid elements we used, as far as available, statistics that showed the most detailed geographical distribution of the animals. The number of animals in an area was then redistributed over the appropriate grid elements proportional to the areas occupied by the different grid elements.

N-production by animals Animals excrete nitrogen by way of faeces and urine. This nitrogen is a potential source of NH 3 . In our calculations we made a difference between nitrogen produced during the housing of animals and nitrogen produced when the animals are at grass. This was done while during housing often mixtures of faeces, urine and sometimes straw are obtained; N-losses differ therefore considerably from those from pure faeces and urine. Data about the total N-production (N 1) during housing were taken from CEC (1978a, 1978b) for most countries. For the U.K. we used the information of Nielsen (1984), for Denmark, Norway and Sweden we used the information of Sommer et al. (1984).

Table 1. Total number of animals in the European countries Cattle Albania Austria Belgium Bulgaria Czechoslovakia Denmark F.R.G. Finland France G.D.R. Greece Hungary Ireland Italy Luxemburg Netherlands Norway Poland Portugal Romania Spain Sweden Switzerland Turkey U.K. U.S.S.R.* Yugoslavia Europe

478~

2536 3025 1796~

5131 2873 15,098 1719 23,599 5690 831 ~ 1922 6908 8734 221 5241 971 11,912 1173 6303 4495 1902 1954 16,983 ~ 13,155 42,200 5474 192,324

Pigs 125 3920 5040 3808 7126 9317 22,478 1475 11,711 12,107 1107 9035 1031 8928 68 10,254 687 19,471 2448 12,464 11,263 2677 2071 11 7975 33,100 7867 207,474

Poultry 484 11,371 29,327 41,096 49,212 16,296 83,033 7763 234,131 51,356 29,846 45,397 9903 137,999 121 88,174 5571 67,244 4143 109,244 42,824 11,393 6188 59,660 130,018 385,000 65690 1,724,484

Horses

Sheep

Year

43 35 30 120 44 41 369 20 278 81 420 120 68 273 1 59 25 1734 23 566 242 57 45 784 140 1556 573 7747

914t 326§ 120 11,271 t 990 58 1172 104 14,34611 2220§ 12,669§ 3183 3323t 10,497§ 3 1210 1999 3899 2811§ 17,748§ 16,543t 437 336 70,093t 32,888 21,000§ 7384 238,544

1981 1980 1982 1981 1982 1982 1982 1982 1982 1982 1981 1982 1980 1980 1982 1982 1979 1982 1981 1981 1982 1983 1983 1981 1982 1982 1980

All data in 1000 heads. *Part of the U.S.S.R., includes the U.S.S.R. republics Ukraine White Russia, Georgia, Azerbajdzjan, Lithunia, Moldavia. ' t Includes asses, goats, mules. §Includes goats. 11 Includes asses, goats. ~Includes buffaloes.

Anthropogenic NH 3 emissions in Europe The total amount of N produced during housing is generally given as N produced by way of solid or liquid manure. Furthermore, N 1 is referred to as N present at the moment of applicating the manure, i.e. 2 months after production (CEC, 1978a). Before that a certain amount of N has been lost through nitrification, runoff and NH 3-emission. To account for these losses a correction should be made as proposed by Sommer et al. (1984), thus obtaining a figure which refers to the actual amount of N produced during the housing of animals (N 1, 0 ). Cattle and horses are at grass during a part of the year; sheep very often almost a year. Then N is produced separately by way of faeces (Nr) and urine (Nu)· This N production is estimated by Kolenbrander and de la Lande Cremer (1967) for cattle and horses and by CEC (1978b) and Taiganides (1977) for sheep. In modern agricultural practice, i.e. intensive livestock breeding, most of the poultry and the pigs are housed during their complete lifetime. Thus, for these animal types only N production during housing is considered. Average N productions for different animal types are given in Table 2. These values are weight (or age) weighted means and should be regarded as indications.

NH 3 emission factors N in faeces, urine and manure is partly lost as NH3. Other possible N losses include leaching of nitrate and ammonium, emission of dinitrogen and dinitrogen oxide. Unfortunately only few experiments have been carried out which focussed particularly on the NH3 emission. Most research has been devoted to study the fate of N in the soil. Emission losses, including NH3, in most cases are a closing entry to balance input and output of N in the soil system. Sommer et al. (1984), having evaluated scarce older experiments in which NH 3 losses from manure during storage were examined, propose NH 3 emission factors ranging from 10 to 20% of N 1,0 • Vanderholm (1975) has summarized available literature about losses in relation to different storage methods. Losses ~e­ ported for aerated systems were 30-90% ofNt,o' wh!le anaerobic storage gave rise to losses from 10 to 75 %· As no sufficient information is available about the storage systems in use throughout Eur~pe we. h~ve assumed for the time being a conservative emission factor of 10% for liquid manure (cattle, pigs), 20% for solid poultry manure and 15% for solid horse manure.

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The different factor for poultry manure is based on the findings of Giddens and Rao (1975). They found losses of up to 50% in the case of airdrying of manure, which is a common practice in modern laying-chicken farms. More information is available about the NH 3 emission during and after applying manure to land surfaces. However, emission factors derived from experiments under realistic field conditions differ widely, mainly because of differences in the many variables influencing the emission: kind of manure (liquid/solid), temperature, wind speed, soil and manure pH, surface application or incorporation of manure in the soil. On the other hand there is agreement that most NH 3 is emitted in a time span of 1-2 weeks after applying manure and that the primary source of NH 3 in this period is the mineral part of nitrogen (Nm) in manure. The mineral part is generally assumed to be N in chemically simple forms, like urea, ammonium, nitrate and simple organic N-substances (CEC, 1978a). In general it holds that Nm is 40-50% of N 1 (CEC, 1978a). Adriano et al. (1974) report for synthetic cattle manure mixed with the soil NH 3 -N-losses approaching 50% of N 1 over a period of 16 weeks. Losses were reduced at lower temperature and lower moisture levels in the soil. Beauchamp et al. (1978) measured NH 3 losses between 24 and 33% ofNm over a period of 7 days, again the emission being strongly dependent on temperature. Lauer et al. (1976) report losses from solid cattle manure varying between 61 and 99 %of N m over a period of 5-25 days. Hoff et al. (1981) measured NH 3 losses from liquid swine manure under various conditions. They found losses of 10-50% of N m after surface application. Injection of manure into the soil greatly diminished the emission. On the other hand higher soil and manure pH, as well as increased temperature and windspeed, gave substantial higher emissions: up to 65% of Nm over a 3!-day period. Giddens and Rao (1975) studied NH 3 losses from solid poultry manure after surface application. Losses were 11% of N 1• CEC (1978a) proposes emission factors for liquid manure: 20% of N m if manure is applied on arable land thereby incorporation of manure in the soil assu:Oing, and 32.5% of Nm after applying on grassland. These emission factors are assumed to be applicable in W European agricultural practice.

Table 2. Average N-production by animals (kg N a -I) Nt,O

Nu

Nr

Housing period (y)

32* 10*

40* 13*

13

11

17t 0.48t

2lt 0.60t

5.6 4.3

5.6 9.5

1/2 1 0 2/3

Animal type

NI

Cattle Pigs Sheep§ Horses Poultry

*Assuming liquid manure is produced. t Assuming solid manure is produced. I §Assumed to be the same for goats, asses, mu es.

1

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Table 3. NH 3 emission factors for animals Animal type Cattle Pigs Sheep Horses Poultry

Storage

After application

Faeces

Urine

0.10 X Nt.O* 0.10 x N1,o*

0.4 X Nm§ 0.2 X Nm~

0.05 x Nr

0.40 X Nu

0.15 x N1,0 t 0.20 x N1,0 t

0.15 X Nt 0.20x N1

0.05 x Nr 0.05 x Nr

0.40 X Nu 0.40xNu

*For liquid manure. t For solid manure. § Nm is 40% of N1• Assuming cattle manure is surface applied on grassland (CEC, 1978a). . ~Nm is SO% of N1• Assuming pig manure is applied on arable land with subsequent incorporation into the soil (CEC, 1978a).

Therefore we used the CEC emission factors for liquid manure with the exception that we raised the factor for grassland to 40% of Nm in view of forementioned experimental results. For solid manure (horses, poultry) we used in the absence of extensive experimental support the emission factors from Sommer et al. (1984) for poultry manure (20% of N 1) and from Kolenbrander and de la Lande Cremer (1967) for horse manure (15% of N 1). Faeces and urine produced when animals are at grass also give rise to NH 3 emission. Substantial enrichment of the atmosphere with N-compounds has been observed in the vicinity of areas grazed by animals (Hutchinson and Viets, 1969; Elliot et al., 1971; Luebs et al., 1973, 1974; Denmead et al., 1974; Hutchinson et al., 1982; Ryden and McNeill, 1984). Although atmospheric NH 3 concentrations up to several hundreds of Jlg m -J are reported it is not possible to relate the reported concentrations directly to the amount of N lost from faeces and urine. However Hutchinson et al. (1982), making a rough estimate, state that approximately 50% of N 1 should have volatilized from cattle excrements in the grazing period. Some direct measurement of NH 3 losses from urine are reported by Stewart (1970), Ball et al. (1979) and Sherlock and Goh (1984). Stewart (1970), using cattle urine, reports losses from 25% of Nu with wet soil up to 90% of Nu with dry soil. Ball et al. (1979) studied NH 3 volatilization from sheep urine. Losses of up to 20% of Nu were observed over a period of 18 days; the emission rate was probably reduced by low soil pH. Sherlock and Goh (1984) also studying sheep urine found losses of 12% ofNuin winter and 25% ofNuin summer. Repeated applications to the same spot gave losses of up to 40% of Nu· No results are reported for the NH 3 volatilization from faeces under field conditions, the only estimate being the one given by Kolenbrander and de la Lande Cremer (1967): 5% ofN 1• A summary of the emission factors used in this work is given in Table 3. Table 4 shows the resulting NH 3 emissions for the animal types involved. The emissions shown in Table 4 can be directly applied to calculate

Table 4. NH 3 emission by animals (kg NH3 a- 1 )§ Animal type* Cattle Pigs Sheep Horses Poultry

Storage losses

Application losses

Losses at grass

4.9 1.5

6.3 1.3

7.2

3.8 0.11

3.0 0.15

3.1 2.6

Total 18 2.8 3.1 9.4 0.26

* Same definition as in Table 2. . . §Based ori N production figures in Table 2 and emission factors in Table 3.

approximate NH 3 emissions if the total number of animals in a category is known. However the NH3 emissions in Table 5 are as far as information was available, based upon the' actual age- or weight distri· butions in an animal category. . . s In Table 5 a summary is given for the NH3 emiSSIOn · m · 0 ur from animal wastes in 27 European countnes inventory. NH 3 EMISSION FROM FERTILIZERS

Nitrogenous fertilizer consumption data, emission factors The consumption data for nitrogenous fertilizers were taken from publications of national stati~tical or agricultural organizations. Otherwise informatiOn was taken from FAO (1982b). As there exist many di~er~nt kinds of N-fertilizers, which all have different emiSSI·~ factors, it was important to gather more spec! c information about the use of the several N-fertilizers~s well. In Table 6 the total fertilizer N-consumptio: ~ given as well as the information available to us w 1~ N-fertilizers were actually used in a country. Detal s and references are given in Appendix II. 1 NH 3 emission from N-fertilizers depends on several factors. In a review article Terman (1979) gives severa summarized conclusions: re . mstances.a - NH 3 losses under comparabl e c1rcu 111 in the order ammonium sulphate > ammomu nitrate > ammonium phosphate.

1

Anthropogenic NH3 emissions in Europe

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Table 5• NH 3 em'tsston · ".rom ammal · wastes in Europe (10 3 t NH 3 a-t)

Albania Austria Belgium Bulgaria Czechoslovakia Denmark Finland France F.R.G. G.D.R. Greece Hungary Ireland Italy Luxemburg Netherlands Norway Poland Portugal Romania Spain Sweden Switzerland Turkey U.K. U.S.S.R.* Yugoslavia Europe

8.7 ~ 53.5 57.4 33.6~

90.7 62.0 31.1 447.5 253.8 103.6 15.1 ~ 35.0 95.7 163.7 4.2 87.1 18.7 216.8 21.3 114.0 81.3 33.2 41.4 393.9~

179.6 768.0 106.6 3517

0.4 5.2 10.7 10.8 20.2 20.2 4.5 25.6 47.7 34.3 2.9 25.6 2.0 19.5 0.1 21.5 1.9 55.1 6.9 35.1 31.8 7.6 4.2 < 0.1 14.4 93.7 14.7 516

0.6 2.5 5.1 10.6 12.8 4.0 2.3 48.8 20.0 13.3 7.8 11.8 2.1 35.2 < 0.1 15.9 1.2 17.2 1.1 28.2 11.1 3.0 1.6 15.0 37.2 100.1 16.7 425

0.4 0.3 0.3 1.1 0.4 0.4 0.2 2.6 3.7 0.8 4.0 1.1 0.9 2.5 < 0.1 0.2 0.2 16.4 0.2 5.3 2.3 0.5 0.5 7.2 1.3 19.6 5.4 78

6.0t 0.6§ 0.3 34.6t 3.0 0.2 0.3 44.611 3.5 6.8§ 39.0§ 9.8 9.4t 31.7§

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76000. 57000. 38000 . 19000 . 32

34

TONS/YEAR TONS/YEAR TONS/YEAR TONS/YEAR 36

38

40

42

Fig. 2. NH 3 emission from cattle in Europe in the early 1980s. Grid size approximately 150 x 150 km 2 at 60° N.

REFERENCES

Adewuyi Y. G. and Carmichael G. R. (1982) A theoretical investigation of gaseous absorption by water droplets from S0 2-HN0 3-NH 3-C0 2-HC1 mixtures. Atmospheric Environment 16, 719-729. Adriano D. C., Chang A. C. and Sharpless R. (1974) Nitrogen losses from manure as influenced by moisture and temperature. J. envir. Qual. 3, 258-261. Ball R. D., Keeney D. R., Theobald P. W. and Nes P. (1979) Nitrogen balance in urine-affected areas of a New Zealand pasture. Agron. J. 71, 309-314. Beauchamp E. G., Kidd G. E. and Thurtell G. (1978) Ammonia volatilization from sewage sludge applied in the field. J. envir. Qual. 7, 141-146. Bonis K. (1981) A nitrogenvegyiiletek legkori merlege Magyarorzag fOlott (The atmospheric budget of nitrogen compounds over Hungary). Idojdrds 85, 149-156 (in Hungarian with English summary). Bonis K., Meszaros E. and Putsay M. (1980) On the atmospheric budget of nitrogen compounds over Europe. Idojdrds 84, 57-68. Bottger A., Ehhalt D. H. and Gravenhorst G. (1978)

Atmosphiirische Kreisliiufe von Stickoxiden und Ammoniak. Ber. Kernforschungsanlage Jiilich, Nr. 158H Breemen N. van, Burrough P.A., Velth.~rst E. J., Dobben · 2 F. van, Wit T. de, Ridder T. B. and ReiJnders H. F. R. (198.) Soil acidification from atmospheric ammonium sulphate 10 forest canopy through fall. Science 299, 548-~5.0. British Sulphur Corporation (1983) World Fertilizer Atlas, 7th edition, London. E Buijsman E., Maas H. F. M. and Asman W. A. H. (1984) den gedetailleerde ammoniak-emissiekaart van Nederlan d) detailed ammonia emission map of the Netherlan s Report V-84-20. Institute for Meteorology a~h Oceanography, State University, Utrecht (in Dutch Wit English summary). 985) Buijsman E., Maas H. F. M. and Asman W. A. H; (1 IE 1 Ammonia emission in Europe. Report R-85-1, me· . annex. Institute for Meteorology and 0 ceanography• State University, Utrecht. . 1982) Cass G. R., Gharib S., Peterson M. and TJiden J. W. (. The origin of ammonia emissions to th~ atmosph:Qre~: ft~ urban area. Open File Report 82-6. Environmenta Laboratory, California, Institute of Technology4) USSR Central Statistical Board of the U.S.S.R. (198

d

1

Anthropogenic NH 3 emissions in Europe yearbook 1982, Moscow. Central Statistics Office (1983) Agricultural Statistics 1980 Dublin. ' Commission of the European Communities (1978a) Information on agriculture no. 47, Luxemburg. Commission of the European Communities (1978b) Information on agriculture no. 48, Luxemburg. Danmarks Statistik (1983) Landbrugstatistik 1982, Copenhagen. Dawson G. A. (1977) Atmospheric ammonia from undisturbed land. J. geophys. Res. 82, 3125-3133. Denmead 0. T., Simpson J. R. and Freney J. R. (1974) Ammonia flux into the atmosphere from a grazed pasture. Science 185, 609-610. Department of Agriculture (1984) Northern Ireland Agricultural Statistics 1982, Belfast. Devlet Istatistik Enstitiisii (1982) Tarimsal yapi ve uretim, Ankara. Directia Centrala de Statistica (1983) Anural Statistic al Republicii Socialiste Romania 1982, Bukarest. Elliott L. F. G., Schuman G. E. and Viets F. G., Jr (1971) Volatilization of nitrogen-containing compounds from beef cattle areas. Soil Sci. Soc. Am. Proc. 35, 752-755. EMEP/CCC (1980) Summary report from the chemical coordinating centre for the first phase ofEMEP. Report 4/80. EMEP/CCC (1984) Summary report from the chemical coordinating centre for the second phase of EMEP. Report 2/84. FAO (1982a) FAO production yearbook, Rome. FAO (1982b) Fertilizer yearbook 1981, Rome. Fcderalni Statisticky Urad (1983) Statistical Yearbook of the Czechoslovak Socialist Republic 1983, Prague. Fenn L. B. and Kissel D. E. (1974) Ammonia volatilization from surface applications of ammonium compounds on calceareous soils-11. Effects of temperature and rate of ammonium nitrogen application. Soil Sci. Soc. Am. J. 38, 606-610. Fenn L. B. and Miyamoto (1981) Ammonia loss and associated reactions of urea in calcareous soils. Soil Sci. Soc. Am. J. 45, 537-540. Fenn L. B., Matocha J. E. and Wu E. (1981a) Ammonia losses from surface-applied urea and ammonium fertilizers as influenced by rate of soluble calcium. Soil Sci. Soc. Am. J. 45, 883-886. Fenn L. B., Taylor R. M.and MatochaJ. E. (1981b)Ammonia losses from surface-applied nitrogen fertilizer as controlled by soluble calcium and magnesium: general theory. Soil Sci. Soc. Am. J. 45, 777-781. Forster J. and Lippold H. (1975) Ammoniakverluste bei Harnstolfdiingung-2. Mitteilung: Ermittling von Ammoniakverlusten unter Feldbedingungen in Abhiingigkeit von Witterung. Archiv fiir Acker- und Pflanzenbau und Bodenkunde 19, 631-639. Freyer H. D. (1978) Seasonal trends of NHt and NOj' nitrogen isotope composition in rain collected at Jiilich, Germany. Tellus 30, 83-92. Georgii H. W. and Lenhard U. (1978) Contribution to the atmospheric NH 3 -budget. Pageoph. 116, 385-392. Giddens J. and Rao A. M. (1975) Effect of incubation and contact with soil on microbial and nitrogen changes in poultry manure. J. envir. Qual. 4, 275-278. Harkins J. H. and Nicksic S. W. (1967) Ammonia in auto exhaust. Envir. Sci. Technol. 1, 751-752. Hessisches Statistisches Landesamt (1983) Viehbestiinde am 3. Dezember 1982 in den Hessischen Gemeinden, Wiesbaden. Hoff J. D., Nelson D. W. and Sutton A. L. (1981) Ammonia volatilization of liquid swine manure applied to cropland. J. envir. Qual. 10, 9G-95. . . . Hood A. E. M. (1982) Fertilizer trends in relation to biological productivity within the U.K. Phil. Trans. R. Soc. Lond. B 296, 315-328. Hooker M. L., Peterson G. A. and Sander D. H. (1973)

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Ammonia nitrogen losses from simulated plowing of native soils. Soil Sci. Soc. Am. J. 37, 247-249. Hutchinson G. L. and Viets F. J., jr. (1969) Nitrogen enrichment of surface water by absorption of ammonia volatilized from cattle feedlots. Science 166, 514-515. Hutchinson G. L., Mosier A. R. and Andre C. E. (1982) Ammonia and amine emissions from a large cattle feedlot. J. envir. Qual. 11, 288-293. Instituto Centrale di Statistica (1981a) Annuario di statistica agraria, Rome. Instituto Centrale di Statistica (1981b) Annuario statistico della zootechnica, pesca e caccla, Rome. Instituto Nacional de Estatistica (1982) Annuario de Estatistica agraria 1981, Lisbon. Instituto Nacional de Estadistica (1983) Annuario Estadistica de Espana 1982, Madrid. Instituto Nacional de Estadistica (1982) Estadisticas agricolas 1981, Madrid. Junge C. E. and Ryan T. G. (1958) Study of the S0 2 oxidation in solution and its role in atmospheric chemistry. Q. Jl R. Met. Soc. 84, 46-55. King L. D. (1973) Mineralization and gaseous loss of nitrogen in soil-applied liquid sewage sludge. J. envir. Qual. 2, 356-358. Kolenbrander G. J. and de la Lande Cremer L. C. N. (1967) Stalmest en gier: waarden en mogelijkheden (Stable Dung and Vulture: Value and Possibilities). Veenman, Wageningen (in Dutch). Landbouw Economisch lnstituut (1983) Jaarstatistiek van de kunstmeststolfen 1981/1982, The Hague. Larson T.V., Covert D. S., Frank R. and Charlson R. J. (1977) Ammonia in the human airways: neutralization of inspired acid sulfate aerosols. Science 197, 161-163. Lauer D. A., Bouldin D. R. and Klausner S. D. (1976) Ammonia volatilization from dairy manure spread on the soil surface. J. envir. Qual. 5, 134-141. Luebs R. E., Daris K. R. and Laag A. E. (1973) Enrichment of the atmosphere with nitrogen compounds volatilized from a large dairy area. J. envir. Qual. 2, 137-141. Luebs R. E., Daris K. R. and Laag A. E. (1974) Diurnal fluctuation and movement of atmospheric ammonia and related gasses from dairies. J. envir. Qual. 3, 265-269. Maahs H. G. (1983) Kinetics and mechanism of the oxidation of S(IV) by ozone in aqueous solution with particular reference to S0 2 conversion in nonurban tropospheric clouds. J. geophys. Res. 88, 10721-10732. Magyar Kotzponti Statistikai Hivatal (1981) Statistical pocketbook of Hungary, Budapest. Meszitros E. (1981) Atmospheric Chemistry: Fundamental Aspects. Elsevier, Amsterdam. Ministere de !'Agriculture (1983) Annuaire de statistique agricole 1982, Paris. Ministerie van Landbouw (1984) LEI-statistieken 1983, Brussels. National Research Council (1978) Subcommittee on Ammonia. University Park Press, Baltimore. Ministry of Housing, Physical Planning and Environment (1983) Handbook of Emission Factors, part 2: Industrial Sources. Government Publishing Office, The Hague. National Statistical Service of Greece (1984) Agricultural Statistics of Greece 1981, Athens. Oesterreichische Diingerberatungsstelle (1984) Handelsdiingerbeliefering Oesterreichs im Kalenderjahr 1983, Vienna. Oesterreichisches Statistisches Zentralamt (1982) Land- und Forstwirtschaftliche Betriebsziihlung 1980, Vienna. Oesterreichisches Statistisches Zentralamt (1984) Ergebnisse der Landwirtschaftlichen Statistik im Jahre 1982, Vienna. Polish People's Republic Central Statistical Office (1983) Rocznik statystyczny rolnictwa i gospodarki zywnosciowej 1982, Warsaw. Polish People's Republic Central Statistical Office (1984) Results not yet published.

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Robinson E. and Robbins R. C. (1970) Gaseous nitrogen pollutants from urban and natural sources. J. Air Pollut. Control Ass. 20, 303-306. Ryden J. C. and McNeill J. E. (1984) Application of the micrometeorological mass balance method to the determination of ammonia loss from a grazed sward. J. Sci. Food Agr. 35, 1297-1310. Sanders L. (1980) Nitrogen balance experiments under forage maize and grass. J. Sci. Food Agr. 31, 846-847. Savezni Zavod za Statistiku (1981) Stocarstvo i Ribarstvo 1980, Beograd. Schweizerische Bauernsekretariat (1978) Statistische Erhebungen und Schatzungen iiber Landwirtschaft und Ernahrung 1978, Bern. Semb A. and Amble E. (1981) Emission of nitrogen oxides from fossil fuel combustion in Europe. Norwegian Institute of Air Research. Teknisk Rapport nr. 13/81. Service de la Statistique et des etudes economiques (1982) Bullet. du Statec XXVIII, no. 7/82, Luxemburg. Service de la Statistique et des etudes economiques (1983) Bullet. du Statec, XXIX, no. 3/83, Luxemburg. Sherlock R. R. and Gob K. M. (1984) Dynamics of ammonia volatilization from simulated urine patches and aqueous area applied to pasture-!. Field experiments. Fert. Res. 5, 181-195. Slemr F. and Seiler W. (1984) Field measurements of NO and N0 2 emissions from fertilized and unfertilized soils. J. atmos. Chem. 2, 1-24. Soderlund R. (1977) NOx pollutants and ammonia emissions-a mass balance for the atmosphere over NW Europe. Ambio 6, 118-122. Soderlund R. and Svensson B. H. (1976) The global nitrogen cycle. In Nitrogen and Sulphur-Global Cycles (edited by Soderlund R. and Svensson B. H.), SCOPE report 7, Ecol. Bull., Stockholm 22, 23-73. Sommer S., Klausen P. S., Tholstrup Christensen B., Hansen J., Jensen N. and Olsen H. (1984) Beregning afammoniakfordampning fra naturgodning i Danmark (Calculation of the ammonia volatilization from animal manure in Denmark). Miljoministeriet, Center for Jordokologi, Soborg.

Staatlichen Zentralverwaltung fiir Statistik (1983) Statistisches Jahrbuch 1983 der Deutschen Demokratischen Republik, Berlin. Statistical Office of Finland (1983) Annual Statistics of Agriculture 1982, Helsinki. Statistika Centralbymn (1979) Rapporter fran de objektiva Skorddeups Katting arna 1978, Stockholm., Statistika Centralbyrl'm (1984a) Rapporter fr~n landbrukets foretagsregister 1983, Stockholm. Statistika Centralbyr~n (1984b) Rapporter fr~n de objektiva Skorddeups Katting arna, Stockholm. Statistisches Bundesamt (1983a) Viehbestand und tierische Erzeugung 1982, Wiesbaden. Statistisches Bundesamt (1983b) Diingemittelversorgung, Wirtschaftsjahr 1982/83, Wiesbaden. Statistisches Bundesamt (1983c) Landwirtschaftlich genutzte Flachen, Wiesbaden. Statistisches Landesamt Berlin (1983) Statistisches Jahrbuch Berlin 1983, Berlin. Statistisches Landesamt Bremen (1983) Statistische Berichte ciii 1-j/1979 und 1982, Bremen. Statistisches Landesamt Hamburg (1983) Statistische Berichte ciii 1-j/82, Hamburg. Statistisches Landesamt Schleswig-Holstein (1983) Die Viehwirtschaft in Schleswig-Holstein 1982, Kiel. Statistisk Sentralbyr~ (1984) Jordbrukstatistik 1982, Oslo. Stewart B. A. (1970) Volatilization and nitrification of nitrogen from urine under simulated cattle feedlot conditions. Envir. Sci. Technol. 4, 579-582. Taiganides P. E. (ed.) (1977) Animal wastes, London. Terman G. L. (1979) Volatilization losses of nitrogen as ammonia from surface-applied fertilizers, organic amendments, and crop residues. Adv. Agronomy 31, 189-223. Vanderholm D. H. (1975) Nutrient losses from livestock waste during storage, treatment and handling. In Managing Livestock Wastes, pp. 285-286, Proc. lnt. Symp. Livestock Wastes, Am. Soc. Agric. Eng., St. Joseph, Michigan. zavodsky D. and Mitosinkova M. (1984) Estimation of atmospheric budget of nitrogen compounds over Czechoslovakia. ldojdrds 88, 202-209.

Anthropogenic NHJ emissions in Europe

APPENDIX 1: LIVESTOCK STATISTICS

Country

Number of geographical units

Albania Austria Belgium Bulgaria Czechoslovakia Denmark Finland France F.R.G. -Baden-Wiirttemberg -Bayern

1 98 592 1 11 275§ 18 95 5073 1111 2050

-Bremen -Hamburg -Hessen - Niedersachsen - Nordrhein-Westtalen

1 1 426 1030 396

- Rheinland-Pfalz -Saarland - Schleswig-Holstein -West-Berlin G.D.R. Greece Hungary Ireland Italy Luxemburg Netherlands Norway Poland Portugal Rumania Spain Sweden Switzerland Turkey

U.K. -England & Wales -Scotland - Northern Ireland U.S.S.R. Yugoslavia

36 6 15 1 15 52 19 158t 20 13 781 447 49~ 18 ~

40 48~

284 3021 67 951 55 856 40

911

6

References* FAO (1982a) Oesterreichisches Statistisches Zentralamt (1984) Nationaal lnstituut voor de Statistiek (1984) [M] FAO (1982a) Fedenilni Statisticky Urad (1983) Denmarks Statistik (1983) Statistical Office of Finland (1983) Ministere de I'Agriculture (1983) Statistisches Landesamt Baden-Wiirttemberg (1984) [M] Bayerisches Landesamt fiir Statistik und Datenverarbeitung, 1984

[M] Statistisches·Landesamt Bremen (1983) Statistisches Landesamt Hamburg (1983) Hessisches Statistisches Landesamt (1983) Niedersiichsisches Landesverwaltungsamt (1984) [M] Ladesamt fiir Datenverarbeitung und Statistik Nordrhein-Westfalen (1984) [M] Statistiches Bundesamt (1983a) Statistisches Bundesamt (1983a) Statistisches Landesamt Schleswig-Holstein (1983) Statistisches Landesamt Berlin (1983) Staatlichen Zentralverwaltung fiir Statistik (1983) National Statistical Service of Greece (1984) Magyar Kozponti Statistika Hivatal (1981) Central Statistics Office (1983) Instituto Centrale di Statistica (1981b) Service de la Statistique et des etudes economiques (1982, 1983) Centraal Bureau voor de Statistiek (1983) [M] Statistik Sentralbym (1984) [M] Polish People's Republic Central Statistical Office (1984) Instituto Nacional de Estatistica (1982) Directia Centrala de Statistica (1983) Instituto Nacional de Estadistica (1983) Statistika Centralbymn (1984a) Bundesamt fiir Statistik (1984) [M] Devlet lstatistik Enstitiisii (1982) Ministry of Agriculture, Fisheries and Food (1984) [M] Department of Agriculture and Fisheries for Scotland (1984) [M] Department of Agriculture (1984) Central Statistical Board of the U.S.S.R. (1984) Savezni Zarod za Statistiku (1981)

*The symbol [M] after a reference means that statistical data were obtained on magnetic tape. As it deals with very detailed information, no official publication exists. §For cattle, pigs and poultry. 14 for horses and sheep. t For cattle and sheep. 29 for pigs, poultry and horses. ~ 1 for poultry. 11 Not completely considered. See Table I.

1021

Eo BuiJSMAN et al.

1022

APPENDIX 11: FERTILIZER STATISTICS AND ADDITIONAL INFORMATION

Country

n/

Albania Austria

1 8

Belgium Bulgaria Czechoslovakia Finland

18

France

95

F.R.G.

11

G.D.R.

15

Greece Hungary Ireland Italy

1 1 20

Luxemburg

References§ FAO (1982b) Oesterreichische Diingerberatungsstelle (1984) Ministerie van Landbouw (1984) FAO (1982b) FAO (1982b) Hintikka, personal comm. (1984) Ministere !'Agriculture (1983) Statistisches Bundesamt (1983b) Staatlichen Zentralverwaltung fiir Statistik (1983) FAO (1982b) FAO (1982b) FAO (1982b) Instituto Centrale di Statistica (1981a) FAO (1982b)

Additional information agricultural area N-consumption agricultural area

net 8 592

-agricultural area -average fertilizer rate

8

References~

Oesterreichische Statistisches Zentralamt (1984) Nationaal Instituut voor de Statistiek (1984) [M] Fedenilni Statisticky Urad (1983)

agricultural area

327

Statistisches Bundesamt (1983c) Staatlichen Zentralverwaltung fUr Statistik (1983)

agricultural area

15

agricultural area

52

National Statistical Service of Greece (1984)

agricultural area

29

Central Statistics Office (1983)

agricultural area

13

-arable land area - grass land area -fertilizer rates for arable land and grassland

14

Service de la Statistique et des etudes economiques (1983) Buijsman et al. (1984)

Netherlands

14

Landbouw Economish Instituut (1983)

Norway

19

Poland

Statistisk Sentralbyra (1984) FAO (1982b)

agricultural area

49

Polish People's Republic Central Statistical (1983)

Office Portugal

FAO (1982b)

agricultural area

18

Romania

FAO (1982b)

agricultural area

40

Spain

FAO (1982b)

agricultural area

48

Statistika Centralbyran (1984)

-fertilizer rates for 24 different crops -area sown for different crops agricultural area 25

Instituto Nacional de Estatistica ( 1982) Directia Centrala de Statistica (1983) Instituto Nacional de Estadistica (1983) Statistika Centralbyran (1979)

Sweden

24

Switzerland

FAO (1982b)

Turkey U.K.

FAO (1982b) FAO (1982b)

Scotland: -agricultural area U.S.S.R.

9

Yugoslavia

67 55

agricultural area England and Wales: -fertilizer rates for different crops -areas for different crops Northern Ireland: -agricultural area

(1978) . .. .. (1982) Devlet Istatistik Enst1tusu Ministry of Agriculture Fisheries and Food (1984) [M] Hood (1982)

40 Department of Agriculture (1984) 856

Statistical Board of the U.S.S.R. (1984) FAO (1982b)

*Number of areas for which fertilizer consumption data were available. which the NH 3 emission from fertilizers was calculated. § References for nd. 1) References for "c·

t Number of areas for

Schweizerische Bauernsekratariat

Department of Agriculture and Fisheries for Scotland (1984)