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Reactive and Non-reactive Species of in Atmospheric Emission Inventories – A Review

Stefan Reis, Mark Sutton Centre for Ecology and Hydrology (CEH), Edinburgh, Bush Estate, Penicuik, EH26 0QB, United Kingdom [email protected]

Rob Pinder NOAA/Atmospheric Sciences Modeling Division/U.S. Environmental Protection Agency (Mail Drop), Office: E-231G-1, 109 T.W. Alexander Drive, Research Triangle Park, NC 27711

Meigen Zhang, Gao lijie Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, People’s Republic of China 2

Nitrogen pollution starts with N2 Climate change

Nitrate Ecosystems and Manure biodiversity

Ammonium- Materials NH 4 and N Fertilizer cultural 2 industry heritage

Combustion Human & animal health Sources Chemical/physical interactions Effects

I don't have any solution, but I certainly admire the problem. Ashleigh Brilliant 3 Nitrogen pollution: integral approach FCCC CAP Nitrate Directive WFD Climate change

Nitrate Ecosystems and Manure biodiversity

Ammonium- Nitrate Materials NH 4 and N Fertilizer cultural 2 industry heritage CLRTAP NEC Dir.

IPPC/ NECD Combustion Air Quality Directive Human and animal health Sources Chemical/physical interactions Effects 4 Overview of the main sources and sinks of nitrogen-containing species

Sources N2 NH3 NOx N2O Biogenic emissions from the terrestrial & marine biosphere X X X Decomposition of proteins and from animals X Biomass burning and fossil fuel consumption X X X Agricultural nitrate fertilisation X Lightning X Sinks Wet deposition X X[1] Dry deposition X X Chemical breakdown in the stratosphere X

- [1] as NO3 5 N = food; Energy = N

7000 90 World population milions 80 6000 Agricul. surface milions ha 70 5000 Fertilizer Tgr NOx emissions 60 4000 50

3000 40

Agricultural surface 30 Fertilizers and NOx World population and 2000 20 1000 10 0 0 1850 1900 1950 2000 Year

Carl BoschFritz Haber

Slide courtesy of: Jan Willem Erisman, ECN/Netherlands 6 Effects of reactive nitrogen in the environment

Slide courtesy of: Jan Willem Erisman, ECN/The Netherlands 7 1 Comparison of EU27 emissions of NH3 reported to EMEP and compiled by IIASA for the year 2000 900 EMEP IIASA 800

700

600

500

Gg 400

300

200

100

0 Italy Spain Latvia Ireland Austria Poland France Cyprus Finland Greece Estonia Belgium Bulgaria Sweden Hungary Slovakia Portugal Slovenia Lithuania Romania Denmark Germany Netherlands Luxembourg United Kingdom 1) not showing Malta and Cyprus Czech Republic 8 1 Comparison of EU27 emissions of NOx reported to EMEP and presented in the EDGAR database for the year 2000 3000 EMEP EDGAR EDGAR (excl. biomass burning & international shipping)

2500

2000

1500 Gg

1000

500

0 Italy Spain Latvia Ireland Austria Poland France Cyprus Finland Greece Estonia Belgium Bulgaria Sweden Hungary Portugal Slovakia Slovenia Lithuania Romania Germany Denmark Netherlands Luxembourg United Kingdom Czech Republic Czech 1) not showing Malta and Cyprus 9 1 Comparison of EU27 emissions of N2O reported to UNFCCC and presented in the EDGAR database for the year 2000 350 UNFCCC EDGAR 300

250

200 Gg Gg 150

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0 Italy Spain Latvia Ireland Poland Austria France Finland Greece Estonia Sweden Belgium Bulgaria Portugal Slovakia Hungary Slovenia Lithuania Romania Denmark Germany Netherlands Luxembourg United Kingdom Czech Republic

1) not showing Malta and Cyprus 10

Regional trends in NOx and NH3 emissions based on EMEP (gap-filled ‘expert emissions’ for the EU27), US EPA (NEI Tier1 emissions) and literature assessments for China

25 NOx (EMEP)

20 NH3 (EMEP) -26%

15 NOx (USEPA) -36% Tg 10 NH3 (USEPA)

-18% NOx (China, 5 Tian et al.) -6% NH3 (China, 0 Klimont et al.) 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 2001 2002 2003 2004 2005 11 Indication of uncertainty estimates for greenhouse gases (Source: Olivier et al., 1999) Emission Factor Total Emissions

Emission source category Activity data CO2 CH4 N2O CO2 CH4 N2O Fossil fuel use Fossil fuel combustion S S M M S M M Fossil fuel production S M M - M M - Industry/solvent use Iron & steel production S - S - - S - Non-ferro production S - S - - S - Chemicals production S - S L - S M Cement production S S - - S - - Solvent use M ------Miscellaneous V ------Landuse/waste treatment Agriculture S - L L - L L Animals (excreta/ruminants) S - M L - M L Biomass burning L S M L L L L Landfills L - M - - L - Agricultural waste burning L - L L - L L Uncontrolled waste burning L ------All sources - - - - S M L S = small (10%); M = medium (50%); L = large (100%); V = very large (>100%) "-" not applicable/negligible 12 Evaluation ‰ Sectoral structure and inventory compilation ƒ Some historic differences in sectoral structures for air pollutants and GHGs ƒ Inventories compiled due to reporting obligations (EMEP, UNFCCC) often differ from independent compilations (e.g. EDGAR) in methods and completeness ‰ Different regional trends

ƒ Since the 1990s, downward trends were observed for NOx(-26%/-36%) and moderate reductions of NH3 (-6%/-18%) in the US and in Europe

ƒ Some indication of decoupling of energy demand increase and NOx emissions in China, but based on few figures available ‰ Temporal and spatial resolution ƒ Spatial resolution for air pollutant inventories reflects their regional scale (EMEP 50 × 50 km, EDGAR 1° × 1°) ƒ Temporal resolution not addressed in inventories 13 Summary and Conclusions (I) ‰ “Official” vs. “expert estimates” ƒ Question which dataset is ‘better’ depends on the purpose ƒ Official emission reporting to comply with obligations to national/international protocols and directives ƒ Timely delivery, completeness and correctness varying between countries ƒ Independent estimates can support validation and uncertaintiy assessment, based on transparent methodologies and using best available knowledge on emission factors, activity rates etc. ƒ Datasets for modelling need to be gap filled and of known quality, resp. with quantifiable uncertainty ranges for validation/verification purposes ƒ Inventory quality needs to be fit for the purpose 14 Summary and Conclusions (II) ‰ Past emission trends and uncertain future developments ƒ While downward trends in US and Europe are projected to continue,

developments in power generation may lead to future increases in NOx (e.g. use of domestic coal vs. gas/oil imports)

ƒ Moderate reductions (US, Europe) and increases in NH3 emissions (China) highlight the relevance of NH3 control strategies, with its increasing contribution to acidification and ƒ Current plans in Europe to increase shares of bio-fuels in the energy mix

may lead to reduced CO2 emissions, but N2O emissions could increase and (more than?) offset GWP savings (see Crutzen et al., 2008) 15 Summary and Conclusions (III) ‰ Towards a full nitrogen balance? ƒ Significant uncertainties still exist in quantifying emissions in particular from

biogenic and natural sources (NOx and N2O from soils, vegetation etc.) ƒ For a fully integrated assessment of nitrogen effects, it is paramount to close the gaps in understanding the ƒ Research underway (NitroEurope IP, European Nitrogen Assessment, INI, ...) with the aim to achieve this ƒ Closing the N balance is the key challenge in order to make progress towards integrated management of the nitrogen cycle 16

Thank you for your attention 17 Acronyms and links

EMEP European Monitoring and Evaluation Programme www.emep.int

UNECE United Nations Economic Commission for Europe www.unece.org CLRTAP UNECE Convention on Long-Range Transboundary Air Pollution www.unece.org/env/lrtap/ExecutiveBureau/welcome.html NEC(D) EC National Emission Ceilings (Directive) http://ec.europa.eu/environment/air/pollutants/ceilings.htm

EC European Commission http://ec.europa.eu IIASA International Institute for Applied Systems Analysis www.iiasa.ac.at UNFCCC United Nations Framework Convention for Climate Change http://unfccc.int

EDGAR International Institute for Applied Systems Analysis www.mnp.nl/edgar

NitroEurope Integrated Project, EC 6th Framework Prog. www.nitroeurope.eu

INI International Nitrogen Initiative www.initrogen.org

ENA European Nitrogen Assessment Report (in preparation) www.nine-esf.org