Biogeosciences www.biogeosciences.net 1726-4170 1726-4189 3 4 2006 10.5194/bg-3-383-2006 http://www.biogeosciences.net/3/383/2006/ http://www.biogeosciences.net/3/383/2006/bg-3-383-2006.html http://www.biogeosciences.net/3/383/2006/bg-3-383-2006.pdf 383 395 2006-08-09 Controls over N₂O, NO_x and CO₂ fluxes in a calcareous mountain forest soil B. Kitzler S. Zechmeister-Boltenstern C. Holtermann U. Skiba K. Butterbach-Bahl Federal Research and Training Centre for Forests, Natural Hazards and Landscape (BFW), Seckendorff-Gudent-Weg 8, Vienna, Austria Sellenyg. 2–4/52, Vienna, Austria Institute of Terrestrial Ecology, Bush Estate, Penicuik, Midlothian EH26 OQB, Scotland Institute for Meteorology and Climate Research, Atmospheric Environmental Research, Forschungszentrum Karlsruhe, Kreuzeckbahnstrasse 19, 82467, Garmisch-Partenkirchen, Germany We measured nitrogen oxides (N₂O and NO_x), dinitrogen (N₂) and carbon dioxide (CO₂) emissions from a spruce-fir-beech forest soil in the North Tyrolean limestone Alps in Austria. The site received 10.6–11.9 kg N ha^−1 y^−1 nitrogen as bulk deposition. Fluxes of nitric oxide (NO) were measured by an automatic dynamic chamber system on an hourly basis over a two year period. Daily N₂O emissions were obtained by a semi-automatic gas measuring system. In order to cover spatial variability biweekly manual measurements of N₂O and CO₂ emissions were carried out in addition. For acquiring information on the effects of soil and meteorological conditions and of N-deposition on N-emissions we chose the auto-regression procedure (time-series analysis) as our means of investigation. Hence, we could exclude the data's autocorrelation in the course of the time. We found that soil temperature, soil moisture and bulk N-deposition followed by air temperature and precipitation were the most powerful influencing parameters effecting N-emissions. With these variables, up to 89% of observed temporal variations of N-emissions could be explained. During the two-year investigation period between 2.5 and 3.5% of deposited N was reemitted in form of N₂O whereas only 0.2% were emitted as NO. At our mountain forest site the main end-product of microbial activity processes was N₂ and trace gases (N₂O and NO) were only of minor importance. Beier, N. and Schneewind, R.: Chemical reactions of gases in tubes of probing systems and their influence on measured concentrations., Ann. Geophys., 9, 703–-707, 1991. Borken, W. and Brumme, R.: Liming practice in temperate forest ecosystems and the effects on CO₂, N₂O and CH₄ fluxes, Soil Use and Management, 13, 251–257, 1997. Brumme, R. and Beese, F.: Effects of liming and nitrogen fertilization on emissions of CO₂ and N₂O from temperate forest, J. Geophys. Res., 97, 12, 851–858, 1992. Brumme, R., Borken, W., and Finke, S.: Hierachical control on nitrous oxide emission in forest ecosystems, Global Biogeochem. Cycl., 13, 1137–1148, 1999. Butterbach-Bahl, K., Gasche, R., Breuer, L., and Papen, H.: Fluxes of NO and N₂O from temperate forest soils: impact of forest type, N deposition and of liming on NO and N₂O emissions, Nutr. Cycl. Agroecosys., 48, 79–90, 1997. Butterbach-Bahl, K., Breuer, L., Gasche, R., Willibald, G., and Papen, H.: Exchange of trace gases between soils and the atmosphere in Scots pine forest ecosystems of the northeastern German lowlands: 1. Fluxes of N₂O, NO/NO₂ and CH₄ at forest sites with different N-deposition, For. Ecol. Manag., 167, 1–3, 123–134, 2002. Conrad, R.: Soil microrganisms as controllers of atmospheric trace tases (H₂, CO, CH₄, OCS, N₂O, NO), Microbiol. Rev., 60, 609–640, 1996. Crutzen, P J.: The role of NO and NO₂ in the chemistry of the troposphere and stratosphere, Annu. Rev. Earth Planet. Sci., 7, 443–472, 1979. Crutzen, P J.: Ozone in the troposphere, in: Composition, Chemistry, and Climate of the Atmosphere, edited by: Signh, H P., Van Nostrand Reinhold, New York, 349–393, 1995. Davidson, E A., Keller, M., Erickson, H E., Verchot, L V., and Veldkamp, E.: Testing a conceptual model of soil emissions of nitrous and nitric oxides, BioScience, 50, 667–680, 2000. Englisch, M. and Starlinger, F.: Waldgesellschaften und Standorte im Bereich der Höhenprofile Achenkirch, FBVA-Bericht, 87, 25–54, 1995. Epron, D., Farque, L., Lucot, E., and Badot, P M.: Soil CO₂ efflux in a beech forest: the contribution of root respiration, Ann. For. Sci., 56, 4, 289–295, 1999. Firestone, M K. and Davidson, E A.: Microbial Basis of NO and N₂O Production and Consumption in Soil, in: Exchange of Trace Gases between Terrestrial Ecosystems and the Atmosphere, edited by: Andreae, M O. and Schimel, D S., John Wiley, New York, 7–21, 1989. Gut, A., Scheibe, M., Rottenberger, S., Rummel, U., Welling, M., Ammann, C., Kirkham, G. A., Kuhn, U., Meixner, F. X., Kesselmeier, J., Lehmann, B. E., Schmidt, W., Müller, E., and Piedade, M. T. F.: Exchange fluxes of NO₂ and O₃ at soil leaf surfaces in an Amazonian rain forest, J. Geophys. Res., 107, 8060, doi:10.1029/2001JD000654, 2002. Härtel, E., Zechmeister-Boltenstern, S., and Gerzabek, M.: Gaseous nitrogen losses from a forest site in the north Tyrolean limestone alps, Environm. Sci. Poll. Res., Special Issue 2, 23–30, 2002. Herman, F., Smidt, S., Englisch, M., Feichtinger, F., Gerzabek, M., Haberhauer, G., Jandl, R., Kalina, M., and Zechmeister-Boltenstern, S.: Investitations of nitrogen fluxes and pools on a limestone site in the Alps, ESPR – Environm. Sci. Poll. Res., 46–52, 2002. Holtermann, C.: A transportable system for the on-line-measurement of NO_x (NO, NO$_2)$-emission from soils, Die Bodenkultur, 47, 235–244, 1996. Howard, D M. and Howard, P J.: Relationships between CO₂ evolution, moisture content and temperature for a range of soil types, Soil Biol. Biochem., 25, 1537–1546, 1993. IAEA: Manual on measurements of methane and nitrous oxide emissions from agriculture, International Atomic Energy Agency, Vienna, 90, 1992. IPCC: Climate Change 2001: The Scientific Basis. Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel of Climate Change, in: Cambridge University Press, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., Noguer, M., Van der Linden, P. J., and Xiaosu, D., Cambridge, UK and New York, NY, USA, 881p., 2001. Johansson, C.: Field measurements of emission of nitric oxide from fertilized and unfertilized forest soils in Sweden, J. Atmos. Chem., 1, 429–442, 1984. Kandeler, E.: Ammonium and Nitrate, in: Methods of Soil Biology, edited by: Schinner, F., Öhlinger, T., Kandeler, E., and Margesin, R., Springer, Berlin, 406–410, 1995. Kitzler, B., Zechmeister-Boltenstern, S., Holtermann, C., Skiba, U., and Butterbach-Bahl, K.: Nitrogen oxides emission from two beech forests subjected to different nitrogen loads, Biogeosciences, 3, 293-310, 2006. Klemedtsson, L., Hanson, G., and Mosier, A.: The use of acetylene for the quantification of N₂ and N₂O production from biological processes in soils, in: Denitrification in soil and sediment, edited by: Sorensen, J. and Revsbech, N P., Plenum Press, 167–180, 1990. Li, C., Aber, J D., Stange, F., Butterbach-Bahl, K., and Papen, H.: A process-oriented model of N₂O and NO emission from forest soils,1, Model development, J. Geophys. Res., 105(4) 4369–4384, 2000. Lovett, G M., Weathers, K C., and Arthur, M A.: Control of nitrogen loss from forested watersheds by soil carbon: Nitrogen ratio and tree species composition, Ecosys., 5, 712–718, 2002. Ludwig, J.: Untersuchungen zum Austausch von NO und NO₂ zwischen Atmosphäre und Biosphäre, PhD Thesis, University of Bayreuth, 251, 1994. Ludwig, J., Meixner, F X., Vogel, B., and Förstner, J.: Soil-air exchange of nitric oxide: An overview of processes, environmental factors, and modeling studies, Biogeochemistry, 52, 225–257, 2001. MacDonald, J., Skiba, U., Sheppard, L. J., Ball, B C., Roberts, J D., Smith, K A., and Fowler, D.: The effect of nitrogen deposition and seasonal variability on methane oxidation and nitrous oxide emission rates in upland spruce plantation and moorland, Atmos. Environ., 31, 22, 3693–3706, 1997. Meixner, F. X., Fickinger, T., Marufu, L., Serca, D., Nathaus, F.J., Makina, E., Mukurumbira, L., and Andreae, M. O.: Preliminary results on nitric oxide emissions from southern African savannah ecosystem, Nutr. Cycl. Agroecosys., 48, 123-138, 1997. Merino, A., Pérez-Batallón, P., and Macías, F.: Responses of soil organic matter and greenhouse gas fluxes to soil management and land use changes in a humid temperate region of southern Europe, Soil Biol. Biochem., 36, 917–925, 2004. Mogge, B., Kaiser, E.A. and Munch, J.C.: Nitrous oxide emissions and denitrification N-losses from forest soils in the Bornhöved lake region (Northern Germany), Soil Biol. Biochem., 30, 703–710, 1998. Mutsch, F.: Bodenchemische Charakterisierung des Mühleggerköpfls im Rahmen einer Untersuchung über Stickstoff-Flüsse in den Norditoler Kalkalpen, FBVA Berichte, 116, Wien, 33–40, 2001. NADP: National Atmospheric Deposition Program 2001 Summary, NADP Report, Illinois State Water Survey, Champaign, IL, 2002. Papen, H. and Butterbach-Bahl, K.: A 3-year continuous record of N-trace gas fluxes from untreated and limed soil of a N-saturated spruce and beech forest ecosystem in Germany: I. N₂O-emissions, J. Geophys. Res., 104, 18 487–18 503, 1999. Pilegaard, K., Hummelshoj, P., and Jensen, N O.: Nitric oxide emission from a Norway spruce forest floor, J. Geophys. Res., 104, 3433–3445, 1999. Raich, J W. and Schlesinger, W H.: The global carbon dioxide flux in soil respiration and its relationship to vegetation and climate, Tellus, 44B, 81–99, 1992. Remde, A., Ludwig, J., Meixner, F. X., and Conrad, R.: A study to explain the emission of nitric oxide from a marsh soil, J. Atmos. Chem., 17, 249-275, 1993. Rummel, U., Ammann, C., Gut, A., Meixner, F. X., and Andreae, M. O.: Eddy covariance measurements of nitric oxide flux within an Amazonian rain forest, J. Geophys. Res., 107(D20), 8050, doi:10.1029/2001JD000520, 2002. Schimel, D. S. and Weintraub, M. N.: The implications fo exoenzyme activity on microbial carbon and nitrogen limitation in soil: a theoretical model, Soil Biol. Biochem., 35, 549–563, 2003. Schindlbacher, A., Zechmeister-Boltenstern, S., and Butterbach-Bahl K.: Effects of soil moisture and temperature on NO, NO₂ and N₂O emissions from forest soils, J. Geophys. Res., 109, 1–12, 2004. Sharma, S., Szele, Z., Schilling, R., Munch, J. C., and Schloter, M.: Influence of freeze-thaw on the structure and function of microbial communities and denitrifying population in soil, Appl. Environm. Microbiology, 72, 3, 2148–2154, doi:10.1128/AEM.72.3.2148-2154.2006, 2006. Simek, M. and Cooper, J E.: The influence of soil pH on denitrification: progress towards the understanding of this interaction over the last 50 years, Eur. J. Soil Sci., 53, 3, 345–354, 2002. Skiba, U., Pitcairn, C E R., Sheppard, L J., Kennedy, V H., and Fowler, D.: The influence of atmospheric N deposition on nitrous oxide and nitric oxide fluxes and soil ammonium and nitrate concentrations, Water, Air Soil Poll., Focus 4, 37–43, 2004. Smidt, S., Herman, F., Grill, D., and Guttenberger, H.: Studies of ecosystems in the Limestone Alps – "Achenkirch Altitude Profiles", Phyton, 36, Horn, Austria, 1996. Smith, K A. Ball, T., Conen, F., Dobbie, K. E., Massheder, J., and Rey, A.: Exchange of greenhouse gases between soil and atmosphere: interactions of soil physical factors and biological processes, Eur. J. Soil Science, 54, 4, 779–791, 2003. Tang, Y. S., Cape, J. N., and Sutton, M. A.: Development and types of passive samplers for monitoring atmospheric NO₂ and NH₃ concentrations, The Scientific World, 1, 513–529, 2001. Teepe, R., Brumme, R., and Beese, F.: Nitrous oxide emissions from soil during freezing and thawing period, Soil Biol. Biochem., 33, 1269–1275, 2001. Tietema, A. and van Dam, D.: Calculating microbial carbon and nitrogen transformations in acid forest litter with $^15$N enrichment and dynamic simulation modelling, Soil Biol. Biochem., 28, 953–965, 1996. Van Cleemput, O. and Samater, A H.: Nitrite in soils: accumulation and role in the formation of gaseous N compounds, Fertil. Res., 45, 81–89, 1996. Van Dijk, S M., Gut, A., Kirkman, G A., Meixner, F X., and Andreae, M O.: Biogenic NO emissions from forest and pasture soils: Relating laboratory studies to field measurements, J. Geophys. Res., 107, 8058, doi:10.1029/2001JD000358, 2002. Venterea, R T., Groffman, P M., Verchot, L V., Magill, A H., Aber, J D., and Streudler, P A.: Nitrogen oxide gas emissions from temperate forest soils receiving long-term nitrogen inputs, Global Change Biol., 9, 346–357, 2003. Vermoesen, A., de Groot, C., Nollet, L., Boeckx, P., and Van Cleemput, O.: Effect of ammonium and nitrate application on the NO and N₂O emission out of different soils, Plant Soil, 181, 153–162, 1996. WHO: Updating and revision of the air quality guidelines for Europe, Les Diablerets, 1995. Williams, E J., Hutchinson, G L., and Fehsenfeld, F C.: NO_x and N₂O emissions from soil, Global Biogeochem. Cycl., 6, 351–388, 1992. Wolf, I. and Brumme, R.: Dinitrogen and nitrous oxide formation in beech forest floor and mineral soils, Soil Sci. Soc. Amer. J., 67, 1862–1868, 2003. Yamulki, S., Harrison, R M., Goulding, K W T., and Webster, C P.: N₂O, NO and NO₂ fluxes from a grassland: Effect of soil pH, Soil Biol. Biochem., 29, 1199–1208, 1997. Zechmeister-Boltenstern, S., Hahn, M., Meger, S., and Jandl, R.: Nitrous oxide emissions and nitrate leaching in relation to microbial biomass dynamics in a beech forest soil, Soil Biol. Biochem., 34, 823–832, 2002.