Spatially-differentiated atmospheric source–receptor relationships for nitrogen oxides, sulfur oxides and ammonia emissions at the global scale for life cycle impact assessment

This paper aims to advance regional worldwide source–receptor relationships, providing fate factors for acidifying and eutrophying air emissions (NOx, HNO3, SO2, SO4 and NH3) to be used within life cycle impact assessment. A simulation for the reference year 2005 of the three-dimensional global scale tropospheric GEOS-Chem model was used as the basis of a novel methodological approach to derive source–receptor matrices (SRMs) whose elements are fate factors at a global 2° × 2.5° grid. This new approach makes it possible to assess the impact of transboundary emissions while maintaining regional scale emission differentiation. These 2° × 2.5° grid resolution fate factors were later aggregated at continental and country resolutions using emission weighting. Continental fate factor results showed that 50–70% of nitrogen oxides (NOx, HNO3) and sulfur oxides (SO2, SO4) and approximately 80% of ammonia (NH3) emissions will deposit on the same continent. Results showed that the developed fate factor derivation approach was within a ±10% agreement with GEOS-Chem simulations in which fate factors were determined by withdrawing the regional emission inventory over Canada and in ±50% agreement with current state-of-the-art LCIA fate factors (calculated with the European Monitoring and Evaluation Programme (EMEP) model). The SRMs outlined in this paper facilitate further modeling developments without having to run the underlying tropospheric model, thus opening the door to the assessment of the regional life cycle inventories of a global economy.

► We provide an approach to estimate regional fate factors at a global scale.
► Transboundary impacts can now be evaluated in life cycle impact assessment (LCIA).
► We favorably compared the approach results with direct GEOS-Chem outputs.
► The uncertainties and limitations of the approach are acceptable for LCIA purposes.