Long-term effects of changing atmospheric pollution on throughfall, bulk deposition and streamwaters in a Mediterranean forest.

The abatement programs implanted in Europe to reduce SO2, NO2 and NH3 emissions are here evaluated by analyzing the relationships between emissions in Spain and neighboring countries and atmospheric deposition in a Mediterranean forest in the Montseny mountains (NE Spain) for the last 3decades. A canopy budget model was applied to throughfall data measured during a period of high emissions (1995-1996) and a period of lower emissions (2011-2013) to estimate the changes in dry deposition over this time span. Emissions of SO2 in Spain strongly decreased (77%) and that was reflected in reductions for nssSO4(2-) in precipitation (65% for concentrations and 62% for SO4(2)-S deposition). A lower decline was found for dry deposition (29%). Spanish NO2 emissions increased from 1980 to 1991, remained constant until 2005, and decreased thereafter, a pattern that was paralleled by NO3(-) concentrations in bulk precipitation at Montseny. This pattern seems to be related to a higher share of renewable energies in electricity generation in Spain in recent years. However, dry deposition increased markedly between 1995 and 2012, from 1.3 to 6.7 kg ha(-1) year(-)(1). Differences in meteorology between periods may have had a role, since the recent period was drier thus probably favoring dry deposition. Spanish NH3 emissions increased by 13% between 1980 and 2012 in Spain but NH4(+) concentrations in precipitation and NH4(+)-N deposition showed a decreasing trend (15% reduction) at Montseny, probably linked to the reduction ammonium sulfate and nitrate aerosols to be scavenged by rainfall. NH4(+)-N dry deposition was similar between the compared periods. The N load at Montseny (15-17 kg ha(-1)y ear(-1)) was within the critical load range proposed for Mediterranean sclerophyllous forests (15-17.5 kg ha(-1) year(-1)). The onset of N saturation is suggested by the observed increasing N export in streamwaters.