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Trends in Surface Water Chemistry in Acidified Areas in Europe and North America from 1990 to 2008

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In this article, the authors analyzed trends in surface water chemistry of 173 acid-sensitive sites from 12 regions in Europe and North America and demonstrated that chemical recovery was demonstrated in the form of positive trends in pH and/or alkalinity and acid neutralizing capacity (ANC).

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Article (refereed) - postprint
Garmo , Øyvind A.; Skjelkvåle, Brit Lisa; de Wit, Heleen A.; Colombo, Luca;
Curtis, Chris; Fölster, Jens; Hoffmann, Andreas; Hruška , Jakub; gåsen,
Tore; Jeffries, Dean S.; Keller, W. Bill; Krám, Pavel; Majer, Vladimir; Monteith,
Don T.; Paterson, Andrew M.; Rogora, Michela; Rzychon, Dorota;
Steingruber, Sandra; Stoddard, John L.; Vuorenmaa, Jussi; Worsztynowicz,
Adam. 2014. Trends in surface water chemistry in acidified areas in
Europe and North America from 1990 to 2008. Water, Air, and Soil
Pollution, 225 (3), 1880. 14, pp. 10.1007/s11270-014-1880-6
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1
Trends in Surface Water Chemistry in Acidified Areas in
Europe and North America from 1990 to 2008
Øyvind A. Garmo*
1
, Brit Lisa Skjelkvåle
1
, Heleen A. de Wit
1
, Luca Colombo
2
, Chris Curtis
3
,
Jens Fölster
4
, Andreas Hoffmann
5
, Jakub Hruška
6, 7
, Tore Høgåsen
1
, Dean S. Jeffries
8
, W.
(Bill) Keller
9
, Pavel Krám
6
, Vladimir Majer
6
, Don T. Monteith
10
, Andrew M. Paterson
11
,
Michela Rogora
12
, Dorota Rzychon
13
, Sandra Steingruber
14
, John L. Stoddard
15
, Jussi
Vuorenmaa
16
, Adam Worsztynowicz
13
1
Norwegian Institute for Water Research, Oslo, Norway
2
University of Applied Sciences of Southern Switzerland, Canobbio, Switzerland
3
GAES, University of the Witwatersrand, Johannesburg, South Africa
4
Swedish University of Agricultural Sciences, Uppsala, Sweden
5
Umweltbundesamt, Dessau, Germany
6
Czech Geological Survey, Prague, Czech Republic
7
Global Change Research Centre, Academy of Sciences of the Czech Republic, Brno, Czech
Republic
8
National Water Research Institute, Burlington, ON, Canada
9
Laurentian University, Sudbury, ON, Canada
10
NERC Centre for Ecology & Hydrology, Lancaster Environment Centre, United Kingdom
11
Ontario Ministry of Environment, Dorset, ON, Canada
12
CNR Institute of Ecosystem Study, Verbania Pallanza, Italy
13
Institute for Ecology of Industrial Areas, Katowice, Poland
14
Ufficio aria, clima e energie rinnovabili, Bellinzona, Switzerland
15
US Environmental Protection Agency, Corvallis, OR, USA
16
Finnish Environment Institute, Helsinki, Finland
*Corresponding author. Contact details:
Norwegian Institute for Water Research (NIVA)
Sandvikaveien 59, N-2312 Ottestad, Norway
Telephone. (+47) 91724722, Fax. (+47) 62576653
Email. oga@niva.no
Manuscript
Click here to download Manuscript: Trends in surface water chemistry; revised.doc
Click here to view linked References

2
Abstract
1
Acidification of lakes and rivers is still an environmental concern despite reduced emissions of
2
acidifying compounds. We analysed trends in surface water chemistry of 173 acid-sensitive sites from
3
12 regions in Europe and North America. In 11 of 12 regions, non-marine sulphate (SO
4
*) declined
4
significantly between 1990 and 2008 (-15% to -59%). In contrast, regional and temporal trends in
5
nitrate were smaller and less uniform. In 11 of 12 regions, chemical recovery was demonstrated in the
6
form of positive trends in pH and/or alkalinity and/or acid neutralizing capacity (ANC). The positive
7
trends in these indicators of chemical recovery were regionally and temporally less distinct than the
8
decline in SO
4
*, and tended to flatten after 1999. From an ecological perspective, the chemical quality
9
of surface waters in acid-sensitive areas in these regions has clearly improved as a consequence of
10
emission abatement strategies, paving the way for some biological recovery.
11
12
13
14
Keywords: acid deposition; surface waters; trend analysis; monitoring network; chemical recovery
15
16
17
18

3
1. Introduction
19
Over the past 30 years, acid  has
20
received considerable attention as an international environmental problem in Europe and
21
North America (Likens et al. 1979). Polluted air masses containing sulphur and nitrogen
22
compounds travel long distances across national boundaries. Acidifying compounds thus
23
affect surface waters, groundwaters and acid sensitive soils far beyond their country of origin.
24
Acidification of the environment has lead to fish death and extinction of fish populations
25
(Haines and Baker 1986), soil acidification (Matzner and Murach 1995), and reduced forest
26
vitality (Fischer et al. 2007). Recently, deposition of reactive nitrogen has also been shown to
27
pose a threat to remote terrestrial and aquatic ecosystems through nutrient enrichment (Lepori
28
and Keck 2012; Stevens et al. 2011; Phoenix et al. 2012).
29
The Convention on Long-Range Transboundary Air Pollution (CLRTAP) came into effect in
30
1983 to control air pollutant emissions in Europe and North America, and thereby improve
31
the environmental status of natural ecosystems. Under the CLTRAP, international cooperative
32
monitoring programmes were initiated to assess the impact of atmospheric pollution on
33
ecosystems. For surface waters, the International Cooperative Programme on Assessment and
34
Monitoring Effects of Air Pollution on Rivers and Lakes (ICP Waters) has been an important
35
contributor documenting the effects of the implemented Protocols under CLRTAP since 1985
36
(Kvaeven et al. 2001).
37
The ICP Waters programme is designed to assess, on a regional basis, the degree and
38
geographical extent of acidification of surface waters. The collected data provide information
39
on dose/response relationships for a wide range of acid-sensitive lakes and streams under
40
varying deposition regimes by correlating changes in acidic deposition with the physical,
41
chemical and biological status of lakes and rivers. Data collected by various monitoring
42
schemes are integrated and interpreted, and inter-laboratory quality control systems are run to
43
ensure data are comparable across participating countries. Previous trend analyses of ICP
44
Waters data on surface water chemistry have provided important indications of the geographic
45
extent of acidification and recovery of lakes and streams for the 1980s (Newell and Skjelkvåle
46
1997), the 1980s and 1990s (Stoddard et al. 1999), and up to the start of 2000 (Skjelkvåle et
47
al. 2005; Skjelkvåle et al. 2001). Early assessments provided little evidence for chemical
48
recovery during the 1980s. Subsequently, however, patterns of widespread chemical recovery
49

4
became clear during the 1990s, as indicated by reduced sulphate (SO
4
) concentrations and
50
increases in pH and alkalinity. The reduction in sulphur deposition is considered to be the
51
main driver of the improved acidification status of surface waters and is also substantiated by
52
catchment input output budgets (Prechtel et al. 2001) and acidification models (Jenkins et
53
al. 2003).
54
Whether continued reduction in emissions of sulphur and nitrogen will lead to further
55
improvement of surface water quality in acid-sensitive regions, sufficient to sustain biological
56
recovery, depends on a number of factors (Wright et al. 2005). In some regions, base cations
57
have declined at a similar or greater rate than SO
4
, preventing chemical recovery (Skjelkvåle
58
et al. 2005; Stoddard et al. 1999). Catchments continue to be enriched by nitrogen deposition
59
with possible consequences for enhanced leaching of nitrate (NO
3
) (Curtis et al. 2005;
60
Moldan et al. 2006; Oulehle et al. 2008; Stoddard et al. 2001), especially under climate
61
change. Additionally, widespread increases in concentrations of dissolved organic carbon
62
(DOC) have also been documented and related to changes in atmospheric chemistry, most
63
prominently the decline in sulphur deposition (Monteith et al. 2007). The increase in DOC
64
may dampen expected reductions in acidity as humic substances are naturally acidifying
65
agents (Erlandsson et al. 2011). Thus, ground truth data on the environmental status and
66
recovery of acid-sensitive surface waters remain important for assessing the effects of
67
emission controls.
68
Here, we report trends in key variables of surface water chemistry from 173 monitoring sites
69
from 1990 to 2008. Trends for individual sites, as well as aggregated trends by regions are
70
presented.
71
2. Methods
72
2.1 Selection of variables
73
The analysis of surface water response to changing deposition comprises variables that are
74
sensitive to acidification and recovery:
75
Non-marine SO
4
and NO
3
are strong acid anions. As ICP Waters sites are selected to
76
be remote from the influence of direct terrestrial pollution, elevated concentrations
77
largely reflect the combined effects of recent trends in deposition and ecosystem
78

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Frequently Asked Questions (17)
Q1. What contributions have the authors mentioned in the paper "Trends in surface water chemistry in acidified areas in europe and north america from 1990 to 2008" ?

Garmo et al. this paper analyzed surface water chemistry in acidified areas in Europe and North America from 1990 to 2008. 

215While reduced deposition of sulphur is the main driver behind the extensive decline of 216 freshwater SO4*, the controls of NO3 concentration are complex as a result of the 217 biogeochemical cycling of nitrogen in soils. 

The reduction in sulphur deposition is considered to be the 51 main driver of the improved acidification status of surface waters and is also substantiated by 52 catchment input – output budgets (Prechtel et al. 2001) and acidification models (Jenkins et 53 al. 2003). 

The speciation of aluminium is highly dependent on pH, and decreasing 319 trends in Ali concentration are likely to have occurred at strongly acidified sites with 320 decreasing H + concentration across the ICP Waters network. 

If the increase has mainly been driven by reduced acidification, DOC levels are 281 likely to stabilise in the near future, because further reductions in SO4* concentrations are 282 expected to be relatively slight. 

Regional and temporal patterns in changes of SO4* in surface water in North America 204 and Europe were similar to those observed in precipitation, indicating that reduced deposition 205 of sulphur has been the main driver of decreasing SO4* concentrations in surface waters. 

133 Aspects of site selection, water chemistry/biological monitoring and data handling are also 134 described in detail in the manual. 

201 Trend analyses of SO4 in precipitation have indicated substantial decreases of sulphur 202 deposition, especially in the areas that previously received the highest loads (Tørseth et al. 203 2012). 

calculated from sum of base cations (Ca+Mg+Na+K) 91 minus the sum of acid anions (SO4+Cl+NO3), is an approximate surrogate for 92 alkalinity in waters with relatively low concentrations of DOC. 

The sum of non-marine Ca and Mg equivalents comprise the 85 major fraction of non-marine cations at the majority of acid-sensitive monitoring sites, 86 and was therefore used as a surrogate for total non-marine base cation concentration. 

Factors that have been invoked to explain trends 218 include changes in deposition of nitrogen (Curtis and Simpson 2014; Oulehle et al. 2008; 219 Rogora et al. 2012), progressive N saturation (Curtis et al. 2011) and changes in snow cover 220 (Brooks et al. 

The lack of a clear pattern 334 of regional decline in NO3 leaching remains poorly understood, and the potential for gradual 335 nitrogen saturation of catchments, and consequences for these vulnerable systems, remains a 336 concern, especially in areas receiving high deposition. 

While NO3 concentrations have increased slightly, there has been an 240 overall reduction in acid anion concentration and other mechanisms are therefore required to 241 explain this tendency. 

Waters sites selected for trend analysis 105ICP Waters data are provided by national and provincial monitoring programmes in the 106 participating countries. 

The analysis of surface water response to changing deposition comprises variables that are 74 sensitive to acidification and recovery: 75 Non-marine SO4 and NO3 are strong acid anions. 

294All regions, except the Alps, Appalachians and Virginia Blue Ridge, showed decreasing H + 295 concentration between 1990 and 2008 (Table 2). 

The collected data provide information 39 on dose/response relationships for a wide range of acid-sensitive lakes and streams under 40 varying deposition regimes by correlating changes in acidic deposition with the physical, 41 chemical and biological status of lakes and rivers.