Assessing decadal changes in rainwater alkalinity at a rural Mediterranean site in the Montseny Mountains (NE Spain)

Annual volume-weighted mean (VWM) concentrations in rainwater collected at La Castanya (LC, Montseny Mountains, NE Spain) were analysed from 1983 to 2000 to study the temporal trends in precipitation chemistry. and the causes behind the changes. A significant positive correlation was found between annual rainwater SO(4)(2-) concentrations at LC and Spanish SO(2) emissions (r = 0.73 P = 0.0008) both decreasing remarkably during this period. Rainwater alkalinity increased during the period, shifting from negative values at the beginning (VWM in the 5 initial years = -2.7 mueq l(-1)) to alkaline values in recent years (VWM in the 5 final years = 18.0 mueq l(-1)). Stepwise regression analysis indicated that 88% of the variation of alkalinity could be accounted for by the variability of non-marine Ca(2+) and non-marine SO(4)(2-), with a more prominent dependence on Ca(2+). Rains of African provenance were highly enriched in alkalinity and Ca(2+), but no significant increases in their occurrence were found for the study period. Because of the reported higher dust updraft in northern Africa during years of high North Atlantic Oscillation (NAO) index. we also explored the relationship between rainwater variables associated with an African provenance and NAO. Annual precipitation was inversely related to NAO (r = -0.61. P = 0.007). The annual wet deposition of African dust-related elements showed no correlation with NAO, probably because wet deposition of these elements depends on two factors (precipitation and dust updraft) which have opposite behaviour with respect to NAO. We hypothesise that dry deposition of African dust during dry spells (not sampled in this study) might be higher during high NAO-index years. (C) 2002 Elsevier Science Ltd. All rights reserved.