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Liming for the mitigation of acid rain effects in freshwaters: A review of recent
results

Article  in  Environmental Reviews · February 2011


DOI: 10.1139/a05-009

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91

Liming for the mitigation of acid rain


effects in freshwaters: A review of
recent results
Thomas A. Clair and Atle Hindar

Abstract: Acid rain has affected freshwater ecosystems for more than 50 years in much
of northern Europe and North America. The acidification of waters, along with concurrent
reduction in acid neutralization capacity, has caused deleterious changes to aquatic
populations in much of these regions. To reverse some of the changes to aquatic ecosystems,
a number of governmental and nongovernmental groups have applied lime and other
neutralizing substances to streams, rivers, lakes, and catchments in the most affected or most
ecologically valuable regions. We review the scientific literature published since the late
1980s on liming to provide an overview of successes and failures of various approaches. We
discuss the rationale behind liming programs and why certain approaches may not be helpful
in mitigating acidification effects under varying conditions. One of our main conclusions
is that though water chemistry may be restored if only temporarily, aquatic communities
probably will not return to their original states, though targeted fish species can be restored
using active management approaches. The communities restored, however, are usually more
unstable than those from undisturbed, or pre-acidification conditions. We also show that
liming may have to be conducted for 50 to 60 years in some affected locations, which should
affect the choice of approaches used in mitigation.
Key words: acid rain, mitigation, liming, freshwaters, catchments, salmonids.

Résumé : Les pluies acides affectent les écosystèmes d’eau douce du nord de l’Europe et de
l’Amérique du Nord, depuis plus de 50 ans. Dans plusieurs de ces régions, l’acidification des
eaux, ainsi que la réduction concurrente de la capacité de neutralisation des acides, a apporté
des modifications néfastes dans les populations aquatiques. Afin de renverser certaines des
modifications dans les systèmes aquatiques, un nombre de groupes gouvernementaux et
non-gouvernementaux ont appliqué de la chaux, et autres substances neutralisantes, aux
ruisseaux, aux rivières, aux lacs et aux bassins versants dans les régions les plus affectées, ou
les plus importantes écologiquement. Les auteurs passent en revue la littérature scientifique
depuis la fin des années 1980, sur le chaulage, afin de définir les succès et les échecs
de différentes approches. Ils discutent la logique soutenant ces programmes et pourquoi
certaines approches pourraient ne pas être utiles, pour mitiger les effets de l’acidification dans
certaines conditions. Une des conclusions principales est que bien qu’on puisse corriger la
chimie de l’eau, ne fusse que temporairement, les communautés aquatiques ne retourneront

Received 19 February 2005. Revision accepted 29 June 2005. Published on the NRC Research Press Web site
at http://er.nrc.ca/ on 12 August 2005.
T.A. Clair.1 Environment Canada, PO Box 6227, Sackville, NB E4L 1G6, Canada.
A. Hindar. Norwegian Institute for Water Research (NIVA), Televeien 3, N-4879 Grimstad, Norway.
1
Corresponding author (e-mail: tom.clair@ec.gc.ca).

Environ. Rev. 13: 91–128 (2005) doi: 10.1139/A05-009 © 2005 NRC Canada
92 Environ. Rev. Vol. 13, 2005

probablement pas à leur état d’origine, bien les espèces de poisson ciblées puissent être
restaurées avec l’aide de techniques d’aménagement. Cependant, les communautés restaurées
sont généralement moins stables que celles de milieux non-perturbés, ou celles de conditions
antécédentes à l’acidification. Les auteurs montrent également que le chaulage a pu être
pratiqué au cours des 50–60 dernières années dans certaines régions affectées, ce qui devrait
influencer le choix des approches utilisées pour la mitigation.
Mots clés : pluie acide, mitigation, chaulage, eau douce, bassin versant, salmonidé.
[Traduit par la Rédaction]

Introduction
Acid rain was widely recognized to be a serious problem in Europe and eastern North America
beginning in the mid-1970s. Sulfuric and nitric acids are byproducts of metal smelting, power generation,
and transportation and are transported downwind from their sources and are eventually deposited onto
soils and waters. These acids interact with soil matter and soil solutions. In soils with high buffering
capacity, ion exchange will occur with carbonates leading to the release of Ca and Mg into streams and
lakes. Where soil buffering capacity is low, hydrogen and inorganic aluminum ions (Ali ) from alumino-
silicate minerals will be released in drainage waters (Reuss et al. 1987; Kirchner and Lydersen 1995).
The relative importance of soil and water acidification is obviously dependent on initial soil chemistry
that is mostly determined by its underlying bedrock and glaciation history (Shilts 1981), as well as by
the acid deposition history of the soil.
Acid emission controls have been introduced in both Europe and North America since the early
1980s. These have significantly reduced acid deposition to much of the western hemisphere and have
resulted in improvements in water chemistry (Stoddard et al. 1999). Unfortunately as shown by a number
of authors (Clair et al. 2003; Mulder et al. 1991; Reuss et al. 1987; Skeffington and Brown 1992), the
long-term abuse of terrestrial ecosystems is causing some soils and the waters that drain them to recover
very slowly even with acid emission reductions.
In some regions of Europe and North America, the recovery will take several decades to occur in
areas with low soil base saturation. For example, Clair et al. (2004) show that base cations (calcium,
magnesium, potassium) in a number of Nova Scotia Atlantic salmon rivers will not return to pre-
acidification levels for another 60–100 years if all acid deposition ended within the next 50 years, due
to the loss of buffering capacity of already poor soils. Other modeling studies predict similar kinds of
chemical recovery delays for parts of Europe (e.g., Wright and Cosby 2003). One of the consequences
of this very slow recovery of soils and water is that freshwater communities will not return to pre-
acidification conditions for a very long time, if at all, even under the most aggressive pollution reduction
scenarios.
One method used to accelerate ecosystem recovery is by adding base cations in the form of calcite
(lime, calcium carbonate, CaCO3 ) or other buffering substances to the aquatic ecosystems or to the
catchments that drain into them. As will be described below, materials other than lime have also been
used to mitigate acid rain effects. However, since lime is the substance used in most studies, in this paper
we will refer to the addition of buffering substances as “liming” in order to simplify the terminology,
though this is not technically correct.
The most extensive river and stream liming programs have been done in Scandinavia with the main
objective being to optimize ecological results and cost effectiveness of the counter-measures (Henrikson
and Brodin 1995; Hindar 1997).Approximately US$30 million were spent in Sweden and US$15 million
in Norway in 2000. In all, nearly US$170 million have been allocated to this program since the 1980s
in Norway with even more in Sweden.
The liming of lakes, streams, and rivers has been studied experimentally in North America and
Europe for over 20 years. There is an imposing amount of literature describing the results of experimental
liming, as well as a number of reviews of the large-scale Scandinavian projects (e.g., Henrikson and

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Clair and Hindar 93

Brodin 1995). There are also method manuals and summaries that provide practical advice on mitigation
approaches and techniques (Olem 1991). Despite the reviews that already exist, however, there are a
number of reasons that suggest the need for a new synthesis of liming practices and results.
The first is that a considerable amount of new work has been published since the last major reviews
done in 1995. There are also reports describing results from long-term liming projects in North America
as well as in Europe. As there are now projects reporting over 20 years of liming information, we felt
it useful to synthesize their results to determine project successes and limitations, and to see if new
insights could be discerned from the additional information now available. We also thought it useful
to compare results from the various mitigation approaches to provide guidance on the methods most
suitable for various types of applications.
The second reason for a new review is that all of the systematic, long-term liming work has been
done in northern Europe where governments have developed policies to mitigate acidification effects
on ecosystems (Dickson and Brodin 1995; Sandoy and Romundstad 1995). In comparison to the Scan-
dinavian experience, there has been no governmental guidance or approach regarding liming strategies
in North America, despite a number of research studies and pilot projects conducted in Canada and the
United States. The reasons for the lack of governmental policy are economic, geographical, and philo-
sophical, and will be be discussed further below. We felt that a review of recent advances in science,
and to a lesser extent, policy, might provide a useful document to guide in the development of new
ecosystem management approaches in areas outside of Scandinavia, if liming is deemed necessary by
policy makers in those areas.
Third, acid rain mitigation is an issue that is regaining visibility as new research is showing the slow
rate of recovery in a number of regions, even under rapid emission reductions. We felt that because of a
number of new mitigation initiatives being planned and developed by nongovernmental organizations
(NGOs), governments and industry in Canada and the United States (e.g., Hindar 2001), that a new look
at existing studies was necessary to provide better information on approaches, successes, and failures
to proponents of such work.
Fourth, we noted that many of the studies described in this review were research-driven and short-
term in nature. With the exception of the national Norwegian and Swedish programs, most of them
were eventually discontinued. We therefore felt that some emphasis should be made in looking at the
consequences of reacidification when liming efforts were no longer sustained.
Finally, we summarize the small amount of literature that describes the policy approaches that should
drive decision making regarding liming. Considering what we now know about ecosystem changes under
liming and the amount of time needed to lime until it is no longer necessary, when would such mitigation
measures be worthwhile?
To provide a summary of scientific results and some guidance to prospective users of liming tech-
nology, we organized this paper in a logical sequence. First, we discuss in general terms the types of
mitigation approaches that are commonly used and provide some key references that hold more in-depth
information. We felt that there was no point repeating summaries and descriptions well described by pre-
vious authors. We also discuss in general terms the reported advantages, disadvantages, and co-benefits
of each method.
We then reviewed the literature published in the last 15 years that describes results from the various
liming research programs that have been reported over this period. First, we describe results from the
large-scale Scandinavian liming programs, as they provide a good example of a planned, consistent,
and long-term approach. We then summarize results of smaller research projects that may help better
explain the large-scale results. We then describe results from the various liming studies, starting from
those that provide immediate changes to the chemistry of drainage waters, such as in-stream liming, to
the approaches that are more long-term in nature, especially catchment liming. For each approach, we
identify some of the major papers published in recent years and then discuss the reported changes to the
chemistry and ecology of watercourses that were targeted. We then draw general conclusions as to the

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94 Environ. Rev. Vol. 13, 2005

potential of the approaches in sustaining aquatic ecosystems until water chemistry conditions return to
pre-acidification levels.
Our approach was thorough, but not exhaustive, as we felt that there was no point in repeating the
same kinds of results over and over. We decided to concentrate the review on the literature published
in peer reviewed journals and in established technical report series. There is a large amount of “grey
literature” related to mitigation such as data results, methods, and other government and NGO reports.
However, because of the difficulty in accessing them, and their sometimes rudimentary quality standards,
we have decided not to include these into the review unless they contributed novel information.
We describe the main ecological (as opposed to financial) costs and benefits of the approaches
described to see if there are significant differences in outcomes and effectiveness. We also review the
reasons why liming has been used or rejected as a management tool in various situations. We then make
recommendations on how or why acidification mitigation techniques might be used under different
conditions in North America and elsewhere.

Why liming?
The main stated objective to justify liming projects is the protection of aquatic organisms from
the adverse effects of anthropogenic acidification. Ideally, mitigation efforts should attempt to return
conditions to pre-acidification levels to return communities to their original states. In reality, this is
unlikely to occur for a number of reasons. First, it is unlikely that any mitigation approach can return
the water chemistry of a lake, river, or stream to its pre-acidification state, as the initial, unpolluted state
will have been arrived at through a long evolutionary process where bedrock, soils, soil microbes, plants
as well as the seasonal hydrological cycle interactions will have produced a nonsteady state situation
that cannot be easily simulated (Cronan 1985; Rochelle et al. 1989; Taugbol and Neal 1994).
Secondly, the ecosystems modified by acidification will currently be dominated by species more
tolerant to acidity. Recolonization of acid-sensitive organisms will therefore not occur into virgin systems
and thus new species will have to compete for ecological space with populations already in place.
Moreover, as water quality improves, recolonization will occur in a sequential fashion as sensitive
species are gradually re-established. As Yan et al. (2003) show, a number of alternative recolonization
outcomes will be possible, so that it is highly unlikely that aquatic ecosystems will return to their
previous states.
To simplify the assessment of mitigation efforts, approaches are usually targeted to reach specific
outcomes. The most common approach is to control water pH or alkalinity to allow the passage or
successful reproduction of target fish species (Hindar and Henriksen 1992; Bjerknes and Tjomsland
2001), or to simply allow basic survival of populations with unique genetic traits (Snucins et al. 1995;
Gunn and Mills 1998). One example of how this would be done is using the work of Holt et al.
(2003). They calculated the pH value of 6.0 as a threshold where zooplankton populations would
be protected in Ontario. Mitigation in order to return conditions suitable for a background type of
zooplankton community would then require reaching and maintaining a pH of 6 in a lake. A related
technique is to modify water chemistry to reach a “critical chemical value” such as an acid neutralization
capacity (ANC) of >20 µequiv L−1 (Baker et al. 1990; Lien et al. 1996). Moreover, using the ANC
> 20 µequiv L−1 criterion, liming demands may be predicted using geochemical models on a regional
or subcatchment scale so that dosage rates of liming material can be modified as acid deposition is
reduced (Hindar 1997).

Where is liming useful?


The composition of bedrock and thus soils, as well as acid deposition history, determine the degree of
soil and water acidification, and thus the degree of damage to ecosystems. Scandinavia is the European
area most heavily affected by long-range transport of acidifying pollutants. The region has slowly
weathering bedrock and is near large sulfur and nitrogen emission sources. Because of these factors,

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Clair and Hindar 95

thousands of lake and river fish populations have been lost over the past 50 years (Hesthagen et al. 1999;
Tammi et al. 2003), which has led to reduced biological diversity of freshwater systems.
In Norway, Atlantic salmon (Salmo salar) populations and their specific genetic pools have been
eradicated from about 20 rivers (Hesthagen and Hansen 1991). Other parts of Europe that have been
heavily affected are portions of the Czech Republic, which received massive amounts of acid deposition
until the 1990s (Hruska et al. 2002), as well as parts of Scotland (Howells and Dalziel 1992) and Wales
(Edwards et al. 1990) where thin soils overlie poorly weatherable bedrock. Liming to ameliorate acidity
effects in water has been done in Scandinavia, as well as Scotland and Wales and will be described in
our review.
The most heavily acidified area in North America is the Sudbury region that has been subjected to
local smelter effects since the 1880s (Smol et al. 1998; Winterhalder 1995). Acidification stress was
greatly reduced in the mid-1970s and further again in the 1980s as smelting technology improved. The
long-term ecosystem abuse led to a slow recovery of water chemistry and thus aquatic communities
(Gunn and Mills 1998). Other regions in Canada to have been affected and to have a potential need
for remediation are southern Nova Scotia, located on slate and granitic bedrocks with little buffering
capacity (Lacroix 1996; Watt et al. 2000), as well as the Muskoka Lakes region of central Ontario (Dillon
et al. 1987) located on the granitic Canadian Shield. Liming studies have been done in the Sudbury and
Nova Scotia regions. Liming has also been conducted at a number of locations in the United States.
The largest studies were done in the Adirondack Mountain region of northern New York State (Porcella
et al. 1995), an area receiving relatively high acid deposition amounts from the US mid-west and the
urban East Coast. Other, smaller studies have also been done elsewhere and will be described below.

Liming methods
Before discussing specific study results, the main methods used for aquatic ecosystem mitigation, the
main types of compounds used, and the assumptions under which they are selected must be described.
Three major approaches have been used to increase the pH, ANC and reduce Ali concentrations of
surface waters and these are described below in order of the rapidity by which they affect the chemistry
of stream and lake waters.

Addition of buffering materials directly to running waters


The addition of fine particled lime or other buffering minerals directly to stream or river waters
(often referred to as in-stream liming) provides immediate acid neutralization and thus immediate
improvement to water pH and ANC. The general approach is that an acid stream or river is titrated
using equipment (usually called a doser) that delivers a known amount of usually fine grained limestone
powder that is mixed with water to form a slurry (Fig. 1). The lime amounts added are usually controlled
by pH measuring sensors upstream and downstream of the doser. This approach is the most intuitive
of the methods and is widely used. A comprehensive description of the equipment used in these types
of operations is provided by Olem (1991). There were approximately 300 lime dosers in operation in
Sweden in 1993 (Dickson and Brodin 1995), while 20 Atlantic salmon rivers are limed with dosers in
Norway. Depending on the site, there may be between two and eight dosers in a river. Some of these
operations have extended for over 20 years (Fjellheim and Raddum 2001).
There are number of advantages to in-stream dosing. First, streams and rivers known to be important
for fish passage can be directly targeted and their chemistry carefully controlled (Hindar and Henriksen
1992; Bjerknes and Tjomsland 2001). Secondly, pH and calcium content of the target streams can be
varied on a continuous basis to optimum levels in order to protect the species under consideration, as well
as to reduce waste of liming agents. To ensure proper dose control, new techniques for pH-controlled
lime dosing of large rivers were developed (Hindar 1997) and applied on a large scale in the Vikedal
River (Hindar and Henriksen 1992). In 1996 and 1997 this technology was further improved for salmon

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96 Environ. Rev. Vol. 13, 2005

Fig. 1. Idealized illustration of an in-stream dosing operation. An enclosed space (1) contains instrumenta-
tion (2) and lime storage and delivery system (3). A mixing container (4) is connected to the stream where
a lime slurry is discharged. (Courtesy of Miljøkalk AS.)

rivers with catchment areas of 2000–4000 km2 . pH-controlled lime dosing is based on signals from
both upstream and downstream sensors together with an independent dose control system. The system
ensures cost-effective liming and continuous dosing to meet the target pH levels. For example, a steady
pH around a target of 6.2 is produced in Tovdal River by increasing the Ca concentration by 0.5 to
1.0 mg L−1 . Several of the dosers now also have horizontally oriented, built-in silos in order to meet
aesthetic standards.
There are some serious shortcomings to in-stream liming however. The first is that the equipment
needed to properly run a dosing operation is expensive, as is the need for continued maintenance and
the provision of lime. Dosers may also need to be operated year round, depending on the objectives of
the project. In most regions affected by acid rain, they may require operation and maintenance under
very difficult weather conditions so that the high resource requirements may mean that only a limited
number of sites can be protected when funds are limited. Most importantly, in-stream liming may have

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Clair and Hindar 97

to be done for many decades, until catchment soils recover and supply base cations and alkalinity
suitable for sustainable “natural” populations. The long-term need for mitigation may try the patience
of governments and local NGOs who support these initiatives.
Obviously, only waters downstream of the liming site will be affected by water chemistry changes,
and thus fish passage and fish habitat at specified distances below the treatment site will benefit. Dilution
of limed waters by downstream, untreated water courses will reduce the increased ANC and pH effect
with distance from the treatment site depending on the area drained and the applied dose. The most
obvious way of dealing with this problem in order to continuously maintain acceptable chemical levels
is to increase the number of dosers as was done in southern Norway in the Tovdal with five large dosers
and the Mandal Rivers with three large and five smaller ones situated in subcatchments (Hindar et al.
1998).

Addition of buffering materials to stream sediments


One way of ameliorating chemistry conditions in the smaller upstream sites is by the addition of
buffering substances to stream sediments. Unlike the addition of a powder or slurry to rivers, gravel
sized particles of lime or dolomite are placed in streams as water filters, called barriers (Olem 1991).
Dissolution of the particles provides bicarbonate and base cations as water passes through the barrier. The
practical reality of this approach is that the performance of the barriers can decrease drastically within a
few weeks of installation. For example Watt et al. (1984), amongst many other studies, found that lime
particles rapidly became covered with organometallic coatings that greatly reduced lime dissolution,
and thus further amelioration of the water chemistry. Moreover, sites with very vigorous hydrological
events often lost their barriers, as bedload material was moved downstream. Many of the earlier attempts
at using barriers were therefore abandoned relatively quickly due to these problems (Olem 1991).
There is another way of using limestone cobbles in sediments, however, and that is to provide an
improved habitat for the hatching of fish eggs. As salmonids generally lay eggs in stream sediments,
ameliorating the interstitial water acidity can be beneficial for egg survival. Lacroix (1992) has used
this approach in Nova Scotia. A similar approach has been developed in Norway. Marine deposits of
shell sand are found in shallow areas along some coasts. Shell sand has for more than 50 years been
added to stream sediments in Norway to improve spawning sites. Its widespread use and positive effects
on brown trout reproduction seem to stem from the protective effect of pH-increase in the sediment
gravel where the fish eggs are layed. A recently published report evaluates some of the projects and
gives advice on how to add this material (Barlaup et al. 2002).

Liming lake surfaces


A related approach to stream and river dosing is the liming of lake surfaces. This is extensively used
in Scandinavia by the Norwegian (Sandoy and Romundstad 1995) and Swedish (Dickson and Brodin
1995) acid rain mitigation programs. The approach involves the addition of slurried or fine grained lime
directly onto the surface of a lake. It can be done using boats (Fig. 2), applied on ice before melt, or
aerially from airplanes or helicopters (Olem 1991). Lake liming has the advantage of being relatively
cheap and easy to do if adequate access, and its application to a lake usually brings immediate increases
in pH and ANC and a reduction in Ali .
Direct lake liming has some drawbacks, however. Liming products can be rapidly lost, especially
in lakes with high flushing rates (Gubala and Driscoll 1991). Shallow lakes draining large catchments
are most likely to lose their additives rapidly and require frequent reapplications to maintain water
chemistry at required levels (Alenäs et al. 1991). There is also a significant loss of liming material to
lake bottoms by sedimentation unless extremely fine-ground material (mean particle size <0.02 mm)
is used or the lake is very deep (mean depth >50 m) (Sverdrup 1985). Another serious limitation is that
cold, acid snowmelt water from the surrounding terrain does not mix with deeper, buffered lake waters,
but forms a lens at the lake surface on its way out of the catchment (Rosseland and Hindar 1988). As

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98 Environ. Rev. Vol. 13, 2005

Fig. 2. Specialized applicator boat for lake liming. (Courtesy of Miljøkalk AS.)

we shall see later, this implies that the lake biota is not totally protected after lake liming. Moreover,
though lake and downstream sites can be protected if only temporarily, smaller water courses upstream
of lakes, which may contain fish breeding habitat, are not.

Addition of buffering materials to catchments


Another commonly used approach to improving water chemistry is the application of buffering
substances to the catchments that provide water to streams and rivers. Catchment liming is usually done
with helicopters from which specialized application gear is suspended (Fig. 3), or fixed wing aircraft
with agricultural spreaders or fire fighting capabilities (Olem 1991). Three sub-approaches have been
used: whole-catchment liming, liming only the discharge areas along the streams, and wetland liming.
Catchment liming as an alternative to lake and in-stream liming has been done for several reasons.
The first is that it avoids the problems of poorly mixed lake water columns described above. Another
is that the approach is better at detoxifying smaller, remote (low access) streams and tributaries with
significant ecosystems. A third is its low maintenance character, as liming material needs to be spread
at much lower frequency. For example, Dalziel et al. (1994) predicted that catchment liming effects
in their Scottish study area would last for at least 15 years, so that reapplication of lime did not have
to be frequent. Hindar et al. (2003) estimated even longer duration after application of dolomite in a
Norwegian study.
Catchment liming can provide a number of other advantages. First, there is no need for complex
dosing systems that must be intensively maintained. Secondly, the rationale behind catchment liming is
that it partly returns soil base saturation back to previous levels. Another important feature is that limed
catchment soils tend to retain Ali and that there is less water chemistry variation even during extreme
weather conditions and high flow (Hindar 2005). Grieve (1990a) and Fransman and Nihlgaard (1995)
showed that increases in soil ANC were responsible for reducing Ali and other metals in stream waters,
thus further improving conditions for aquatic life.
© 2005 NRC Canada
Clair and Hindar 99

Fig. 3. Helicopter lifting catchment liming delivery system. (Courtesy of Miljøkalk AS.)

The biggest problem associated with catchment liming is the application cost. The amount of lime
needed will vary depending on soil types and conditions, as well as water flow paths and spreading area.
Clymo et al. (1992) estimated the amount of lime needed to recover a Scottish catchment by trial and
error. Other approaches have used model calculations based on field studies. Warfvinge and Sverdrup
(1988) have attempted to quantify the various parts of the catchment liming process by developing a
model used to optimize liming strategies. Their model emphasized three design parameters: amount
and size of liming material as well as the portion of the catchment that is limed. The Integrated Lake-
Watershed Acidification Study model (ILWAS) developed for the Adirondack region of New York State
(Davis and Goldstein 1988) was also used to predict how much limestone would be needed to neutralize
receiving lake waters. This model was a complex empirically derived approach emphasizing transport
of ions through soil layers.

Buffering compounds used in mitigation


There are a number of buffering compounds that have been used in mitigation and these are well
described by Olem (1991, Table 1). The most commonly used is calcite (calcium carbonate, limestone,
CaCO3), which is common in many soils. Because of its use in agriculture, it is easily available, relatively
inexpensive, and has been well studied in the past. It can be acquired in different particle sizes that makes
it amenable for a wide variety of applications that will be discussed further below.
Dolomite (CaMg(CO3 )2 ) closely resembles calcite in its characteristics, has slightly higher buffering
capacity but dissolves more slowly in acid water (Sverdrup 1985). It is also readily available and has
been used in a number of studies (e.g., Gunn et al. 2001; Hindar et al. 1998) though it is mostly used on
catchment soils and not as an addition to water itself. Two other carbonates, sodium carbonate (soda ash,
Na2 CO3 ) and sodium bicarbonate (baking soda, NaHCO3 ), have also been used in test studies (Olem
1991). Both materials are effective at reducing acidity and are often used in water treatment facilities.
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100 Environ. Rev. Vol. 13, 2005

Table 1. Theoretical neutralization equivalents of the main


compounds assessed for mitigation studies. Values are relative to
CaCO3 (from Olem 1991).
Common name Formula % neutralization equivalent
Limestone CaCO3 100
Dolomite CaMg(CO3 )2 109
Sodium carbonate Na2 CO3 94
Sodium bicarbonate NaHCO3 119
Calcined lime (CKD) CaO 179
Calcined dolomite CaO-MgO 207
Hydrated lime Ca(OH)2 135
Caustic soda NaOH 125

However, they are considerably more expensive than calcium-based buffers and have not been used
extensively in field situations.
Mineral oxides (calcium and calcium-magnesium oxides, CaO and CaO-MgO, quicklime or cement
kiln dust (CKD)) are the byproducts of cement manufacture. These are often used to decrease acidity
in water treatment plants, but are difficult to store and apply safely in the field (Olem 1991). Dickson
and Brodin (1995) in Sweden and Baalsrud et al. (1985) in Norway specifically council against their
use in the field, citing potential injury to staff and damage to machinery. Dickson and Brodin also
suggest that careless use or accidental releases can locally “induce harmfully high pH in the water”.
Oxides are especially difficult to use under rainy conditions when hydration can occur in equipment or
in temporary open storage. Calcium (slaked lime, Ca(OH2 )), calcium-magnesium ((CaMg(OH)4 )), and
sodium hydroxide (caustic soda, NaOH) are less likely to react with moisture than the mineral oxides,
but can still potentially cause high pH shock in waters when overapplied. NaOH is commonly used
in water and wastewater treatment, but due to its caustic nature is not recommended for use in natural
situations (Olem 1991).
Silicates such as slag lime, a waste product of metal smelting, have been used experimentally in the
1970s and 1980s but have been rejected because of their high metal contents, which can cause problems
in soil and aquatic populations (Alenäs et al. 1991). Wilander et al. (1995) report on the unsuccessful
use of olivene (Mg2 SiO4 ) in a Swedish catchment application, due to slow dissolution. Finally, there is
currently an experimental application of crushed wollastonite (CaSiO3 ) in one of the Hubbard Brook
calibrated catchments. The objective of the study is to attempt to simulate the buffering capacity of
natural silicate soil–bedrock systems. Likens et al. (2004) report that there was an improvement in
water pH, ANC, and base cations in the study stream though the improvements were only noted during
baseflow conditions. Silicates tend to dissolve much more slowly than carbonate minerals and are thus
less favoured for rapid action.
Sodium silicate (Na2 O·SiO2 ) forms silica lye (Si(OH)4 ) in water. The dissolved Si has been shown
to bind strongly to Ali . This material has recently been studied in several experiments in Norway where
the aim was to detoxify Al faster than by the use of calcite. Results have been promising, and this material
will be tested further in a large-scale study (Åtland et al. 2003). The rational behind this approach is
described by Birchall et al. (1989).

Results from liming studies


Addition of buffering materials directly to running waters
The first large river mitigation project in Norway, the liming of River Audna (catchment area of
450 km2 ), was part of a national liming research project in the period 1979–1985. The river had lost
its native salmon stock in the 1970s, and at the time liming by dosers was felt to be the only way of
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reversing a negative water quality trend. The national project was initiated to see if liming would be a
useful measure for protecting sensitive organisms within suitable ecological, technical, and economic
parameters (Baalsrud et al. 1985). Two large lime dosers have been running on a continuous basis since
1985 at this river using calcite powder with particle sizes of up to 0.2 mm. The lime is continuously
transported from a large silo to a mixing tank, mixed with river water to make slurry, and then fed to the
river by gravity. The long-term liming program in River Audna increased water pH and ANC as well as
reduced Ali in water. This has resulted in salmon catches of 2.6 t in 2001, compared with reported mean
catches of 3.5 t in the period 1879–1892 (Hesthagen and Larsen 2003). Significant improvements in
invertebrate acidification indices have also been documented at this river (Fjellheim and Raddum 1995).
These authors have shown that the liming program is important for improving ecological communities.
They show that the recovery rates for the invertebrate communities also depend on the proximity to
existing refuges for sensitive organisms and in different recolonization rates for different invertebrate
types (Fjellheim and Raddum 1992, 2001).
Research on water chemistry effects for Atlantic salmon smolts has resulted in an awareness of
their extreme sensitivity to even very low concentrations of Ali . With improved knowledge, pH targets
are now being optimized based on the sensitivity of different salmon life stages (Staurnes et al. 1995;
Kroglund and Staurnes 1999). Atlantic salmon catches are rapidly increasing in many of the other limed
Norwegian rivers as well, and are up from almost unmeasurable levels before liming to 10–15 t per
annum in River Bjerkreimselva (Walseng et al. 2001) and River Mandalselva in 2001 (Hesthagen and
Larsen 2003). In some rivers, however, salmon returns are lower than pre-acidification levels due to
new migration obstacles such as dam barriers and lowflow stretches caused by hydroelectric power
generation.
In the rivers Tovdalselva and Mandalselva, attempts to control the genetic pool by establishing a
population from nearby rivers by placing fertilized eggs in the river sediments may have failed. Even
very low numbers of spawners in Tovdalselva produced almost the same number of fries (36% and
47% survival in 2000 and 2001) as did the enhancement program (Barlaup et al. 2003). The river
Mandalselva has also been stocked with hatchery produced offspring (fry) of stray salmon from other
rivers. Strayers from other rivers give rise to fry from populations other than the “locally correct” generic
group and these tend to dominate the population (Haraldstad et al. 2003). Insufficient initial efforts and
starting too late to restock with local fish may explain the problem of ensuring the survival of local
gene pools. However, Hesthagen and Larsen (2003) point out that rivers with stocking programs show
higher densities of salmon fry than rivers with no such enhancement programs, which is still a desirable
objective. Degerman and Appelberg (1992) showed that stream liming did not increase the total number
of fish in streams, though salmonid species did increase in density.
In North America, much less work has been done using stream liming for acid rain mitigation. The
technique is commonly used to correct for acid mine drainage in large parts of the continent, but these are
usually much more severe conditions than can be expected from acid rain (Kleinman 1989). Eggleton
et al. (1996) limed a “soft-water” stream in the southern Appalachian Mountains of the United States
in the late 1980s and showed slight improvements in pH and alkalinity, but no measurable changes
in biological parameters. Their project was marred by a number of technical and equipment problems
that might have contributed to their lack of success in changing water chemistry, and thus the aquatic
community.
In a West Virginia stream system Clayton and Menendez (1996) and Menendez et al. (1996) in-
creased pH from 5.0 to 6.5 using lime additions. They reported that during the 5 years of treatment,
the stream became a suitable habitat for eight fish species, and that sustainable trout populations had
been established with the liming program. They also found, however, that benthic invertebrate numbers
were reduced after liming, compared to those of acidic conditions. They tentatively ascribed the lack
of invertebrate improvement to changes in substrates and increased fish predation. Simmons and Doyle
(1996) and Simmons et al. (1996) limed a stream in north-central Massachusetts in order to increase pH

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from 4.9 to 6.5 and thus enhance fish populations. As with all the other studies, they showed increased
trout population densities with increasing pH, though they could not show enhanced growth rates.
An important stress on aquatic populations in acidified ecosystems is the effect of acid pulses
occurring during vigorous snowmelts or significant runoff events (Christophersen et al. 1984; Davies
et al. 1999). Most long-term, in-stream liming programs are designed to cope with these types of rapid
chemistry changes. One program, however, was designed to operate especially when fish populations
are in the greatest danger of exposure to high acidity levels. Hall et al. (1994) designed a stream liming
program specifically to enhance the survival of early life stages of yellow perch (Perca flavescens), white
perch (Morone americana), blueback herring (Alosa aestivalis), and alewife (Alosa pseudoharengus) in
a Maryland stream during acid episodes caused by high runoff events. Despite their success in improving
water quality during key periods of the fishes’life cycles, they found that this was not sufficient to provide
conditions for sustainable populations.
Overall, most of the studies that have reported results of stream or river liming have shown that they
have been able to bring pH and ANC to the levels at which they were aiming, after a reasonable amount
of equipment adaptation and modification. In most cases, the fish species that were targetted showed
some benefit in terms of population increases or improved reproductive success.
Benthic invertebrate populations, which are perhaps a better indication of overall community di-
versity, have tended to show more mixed results. Herrmann and Svensson (1995) showed no increase
in acid-sensitive benthos in limed Swedish streams. On the other hand, also in Sweden, Lingdell and
Engblom (1995) claimed a return to a “pristine” benthic invertebrate in a stream community post-liming.
Appelberg and Svenson (2001) and Fjellheim and Raddum (2001) have shown improvements, but not
a return to pre-acidification communities in other Scandinavian streams. It is likely that length of the
liming period, as well as a host of other factors such as availability of colonizers and predator pressure,
all have an important role to play in determining the success of liming to assist communities to recover.

Addition of buffering materials to stream sediments


The methods for adding buffering materials to stream sediments or as barriers have been worked out
in the acid mine drainage studies in North America (Skousen et al. 1996). However, there are surprisingly
few recently reported studies on results from this approach for acid rain mitigation in North America
compared to Norway, where the method is widely used, probably because earlier North American studies
showed a poor success rate. Olem (1991) reported on several studies in the United States and Canada that
were conducted in the 1980s where beneficial results lasted only a few weeks. The main reason for the
failures seemed to be that the particles would quickly become coated with organometallic complexes that
would then rapidly reduce their dissolution. This result was also reported by Watt et al. (1984) in Nova
Scotian streams. Lefevre and Sharpe (2002) also found no change in benthic invertebrate communities
and very little in fish in Pennsylvania where they applied limestone sand to a stream bottom.
On the other hand, Hudy et al. (2000) applied limestone sand to a first order stream in Virginia
and found that water chemistry stayed at an improved level for over 44 months. They also found that
transplanted trout survived and reproduced in these small streams, though other, non-game species
survived but did not reproduce. The successful results reported by the Hudy et al. (2000) study may be
due to lower peak flows in their stream compared to the other work reported.
Lacroix (1992, 1996) reported on the application of crushed limestone to sediments in a Nova Scotia
Atlantic salmon stream. He found that there was a small, lasting increase in pH in the limed section
of the brook and downstream lasting over 8 years, though limestone had to be replenished once after
4 years because of washouts during floods. He also found that juvenile Atlantic salmon had greater
chances of surviving low pH episodes in the areas that had been limed.
Downey et al. (1994) added between 8 and 50 t of 150–1000 µm limestone in three Virginia streams.
They improved ANC, reduced total Al and Ali , and increased biota populations downstream of the liming
sites. The main controlling factor in improving water chemistry was thought to be contact time between
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Clair and Hindar 103

stream water and sediment limestone. They calculated that the effect would last between 2 and 5 years
before reapplication was needed.
Use of shell sand in Norway is part of the national operational liming program, but has been poorly
studied using controlled experiments. Barlaup et al. (2002) evaluated shell sand additions done by
landowners and fishing organizations. Shell sand was added upstream of spawning sites. They found
that shell sand particles were easily transported downstream, and needed to be replenished every year
or even several times during the year. However, the increased pH in the spawning gravel was clearly
the result of addition from deposits along the stream.
The difference between the successful and unsuccessful studies may be one of degree and of setting
too ambitious aims. The older studies reported (Olem 1991) were mostly attempting to modify water
chemistry of whole streams. On the other had, Lacroix’s and the Norwegian work were more directed
towards improving localized spawning habitat. Though done on a smaller scale than the older studies,
the spawning site method seems to have been more successful due to the more focussed approach.
As will be shown below, liming of lake sediments where fish eggs were laid was also successful in
producing microhabitat chemistry improvements.

Addition of buffering materials to lakes


Effects on water chemistry
Adding limestone or other neutralizing agents directly into lakes is the most commonly used approach
in aquatic acid rain mitigation. The lake liming concept is relatively simple, as is its application in
the field. Nevertheless, there are obviously a number of considerations that must be dealt with when
deciding on which lakes to lime, as well as when and how to lime, and at what dosage. A good
method for calculating the dosage was developed by Sverdrup (1985). Based on studies in sedimentation
chambers, he estimated dissolution rates for lime powders under different pH, temperature, and water
depth conditions. He also explored how the duration of lake liming operations depended on water
retention time. Once in the sediments, the lime was still contributing to increases in lake water pH and
ANC though at a lower rate (Rosseland and Hindar 1988).
The main loss of buffering material in lake liming is to outlet waters and sediments (Gubala and
Driscoll 1991; Rosseland and Hindar 1988). The loss of added buffering capacity in lakes is obviously
not as rapid as it would be in rivers, where depletion of lime from the application point is immediate.
Nevertheless, it can be quite rapid depending on lake water retention times. Gubala and Driscoll (1991)
report that many acidic Adirondack lakes have retention times of <0.5 years, which make them less
suitable for direct liming.
Edberg et al. (2001) found that liming needed to be repeated every 3 to 5 years in order to maintain
pH between 6.6 and 7.1 in a Swedish lake with a 0.8 year retention time. In contrast, Yan et al. (1995)
show pH being enhanced and maintained at >6 between 4 and 16 years in lakes from the Sudbury area
of Ontario, an area with relatively low rainfall. In Norway, Lake Store Howatn, a 1.1 km2 lake with 0.8
year retention time, needed to be limed every one or two years to maintain acceptable pH levels (Hindar
and Wright2 ).
To place retention times in larger perspective, data from 77 lakes of the Swedish National Lake
Liming Program, located on glaciated terrain, were analyzed by Appelberg and Degerman (1991). They
found that the median water retention time of the group was 2.2 years with a minimum value of 0.1 and
a maximum of 45 years. Wilander et al. (1995) showed that in the Swedish terrain, liming for a target
pH of 6 lasted approximately 2 years in 50% of the lakes they studied. They also found that 98% of their
study lakes would reacidify to below pH 6 within 5 years of a single application. Dickson and Brodin
(1995) analyzed further work of the Swedish National Program and showed a curvilinear relationship
between water retention time and reacidification time. Liming lakes with short retention time for a long
period requires higher doses and is expensive as the loss through the lake outlet is relatively large.
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104 Environ. Rev. Vol. 13, 2005

Norwegian lakes are therefore limed more frequent today than at the start of the liming operations in
the 1980s.
One problem that cannot be remedied by lake liming is that of high acidity episodes, especially
during snow-melt. As noted above, these are common phenomena in the spring in northern temperate
climates and during other high flow events in poorly buffered catchments (Davies et al. 1999). Gubala et
al. (1992) report that the near-shore and upper part of the water column of a limed lake in the Adirondack
region of New York State was dominated by low pH and ANC waters originating in snow-melt waters of
the catchment surrounding the lake. The low pH water was also accompanied by Ali concentrations at
levels high enough to be deleterious to the early life stages of fish. This phenomenon was also reported
by Gunn et al. (1990), Booth et al. (1993) in Ontario, and Barlaup et al. (1998) in Norway. Lake liming
can then be seen not to provide longlasting or complete protection against acid water inputs.
To summarize results of the lake water chemistry modifications reported, it is clear that the lake
liming effect is influenced mostly by the catchment characteristics, especially water retention time as
well as climate and application doses. It is a procedure that needs to be repeated frequently when
retention time is low in order to maintain water chemistry targets. It still does not protect all parts of the
lake, as lighter snowmelt waters, which often drain into lakes, create high acidity and Ali conditions in
littoral areas, as well as in the upper portion of the water column.

Effects to ecosystems
As we show above, the effect of lake liming on water chemistry is dependent on a relatively large
number of physical and chemical factors. A review of the literature reveals that the effects on biological
communities are even more complex. One of the more useful features of lakes is that biota are more
easily studied there than in rivers or streams. They also tend to develop more stable populations than
those in lotic systems that are characterised by more dynamic habitats. Lakes provide stable spawning
and reproductive habitats and thus tend to have larger plant and animal species compositions. Because of
these factors, it is easier to assess the effect of liming lake ecosystems than in rivers or streams. However,
based on a review of the reports that we have assembled, we feel that the trends and generalizations
drawn from lake studies are also applicable to running waters and concentrate our analysis of biological
effects on this environment.
As most liming programs were designed to protect, enhance, or recover fish populations, we will first
review that type of work and then will later analyze the literature for the other parts of the ecosystem.
In Norway, the acidification of Lake Store Hovvatn caused the extinction of lake-spawning brown trout
(Salmo trutta) as early as in the 1920s. The lake was first limed as a test in 1981 (Wright 1985) and then
a long-term liming program was initiated in 1987 when 91 t of calcite were mixed onto the lake surface
by boat (Hindar and Rosseland 1991). Repeated liming has since been done annually or every second
year at between 100 and 200 t per annum (Hindar and Wright 2005).
After each liming, pH first increased, and then gradually decreased over the next 1 or 2 years. The
Ali was always reduced as pH increased, but increased again when pH was reduced. Stocked, lake-
spawning brown trout from a nearby lake successfully lived in the lake most of the time, although the
fish had serious problems when pH decreased to about 4.75 and Ali increased to 120 µg L−1 in 1986
(Barlaup et al. 1994). Lake liming achieved the target pH during the ice-free season and Ali was usually
at acceptable levels during these periods. However, acid meltwater resulted in extremely low survival
of fish eggs in nests at 0.5–1.5 m depths during winter time (Barlaup et al. 1998).
Alenäs et al. (1991) reported on the restocking of brown trout in acidified Lake Lysevatten in SW
Sweden. They showed the fish to be in good condition immediately after liming, though their condition
worsened as the liming effect was reduced. They also reported that no fingerlings, which were introduced
immediately after liming, survived to maturity. This confirmed the great susceptibility of the younger life
stages to acidification and the greater need to protect that important life stage. Saksgård and Hesthagen
(1995) found that after 8 years of liming, char, whitefish, and brown trout populations had not recovered

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in a central Norwegian lake. The lack of liming at stream spawning sites seemed to control fish recovery.
They found that perch was more tolerant of acidification and exhibited good recruitment even before
liming occurred. Hesthagen et al. (2001) also limed a Norwegian lake in 1997–1998 that formerly held
perch populations. They restocked it and three unlimed lakes with perch and found that recruitment was
successful in the limed site, but not in the other highly acidic, clear-water lakes at pH of 4.6–4.7.
A summary of liming effects on 77 Swedish lakes by Appelberg and Degerman (1991) showed
that both initial conditions and habitat diversity affected the composition of fish species after liming.
They showed that after liming had occurred, fish recruitment increased and new fish communities were
formed under improved water chemistry conditions. They were not able to measure the development
of a stable fish community in these lakes, however. As the liming influence was reduced with time,
acid-tolerant species became more dominant and the community again became less diverse. Appelberg
and Svenson (2001) also reported that percid fishes tended to dominate limed lakes, like they did in
circumneutral reference lakes, probably because they were able to outcompete trout species in recolo-
nization. Holmgren (2001) used a semi-quantitative approach relating community and size distributions
in circumneutral, limed, and acidified lakes and found that the limed lakes more closely resembled the
circumneutral ones. Nevertheless, she found that there was too much variability in populations to use
this method to separate acidified from non-acidified conditions.
In North America, lake liming was shown to be successful in assisting the recovery of trout pop-
ulations at the highly acidified Bowland Lake in the Sudbury area (Gunn et al. 1990). Once more,
reproductive success seemed to be the major determinant of trout recovery, though they also noted an
improvement of otolith condition in older trout that could only be due to indirect increases in dissolved
calcium (Casselman and Gunn 1992). Gunn et al. (1990) also noted that the fish community structure
was unstable in the lake following liming, which led them to conclude that the long-term effectiveness
of the treatment was uncertain, as it did not seem that the community would return to a pre-acidification
condition.
This conclusion was probably also influenced by previous results that they reported. Nelson Lake,
another limed lake in this region (Gunn et al. 1988), showed that yellow perch disappeared, lake trout
increased, and smallmouth bass were successfully reintroduced. Upon further examination of the data,
however, the authors felt that improved water chemistry due to acid rain reductions might have had a
larger influence on the population shift than the liming itself. Booth et al. (1993) limed lake sediments
in the Sudbury region at spawning shoals to see if they could improve survival of fish embryos. As
with Lacroix (1996), they were successful in enhancing the survival of early life stages of trout and
considered this approach to be a useful lake management tool.
Another North American lake liming study was reported by Schofield et al. (1991) in Woods Lake
of the Adirondack region of New York State. The lake was limed three times over a 5 year period
to maintain pH and ANC at levels to allow the return of brook trout as an important sport fish in
local lakes. However, despite improved water chemistry conditions, they were unable to maintain a
sustainable trout population in the lake. They ascribed this to increased interspecific competition that
suppressed trout survival rates. Popp et al. (1996) found that in a heavily limed Minnesota lake, minnow
and brook trout populations increased. They suggested that the increase in minnows provided more
feeding opportunities for trout, which then enhanced trout survival. Other factors, such as a fishing ban,
may also have contributed to the improved trout numbers.
An evaluation of lake liming effects on fish reveals a few consistent conclusions. The first general
conclusion is that often, but not always, the targetted fish species show some level of population im-
provement when a lake is limed. Even with good liming efforts though, such as described by Saksgård
and Hesthagen (1995) or Schofield et al. (1991), trout and other “desirable” species may not recover.
The first reason for failure seems to be that there is a different initial species competition environment
in the limed lakes that may deny ecological space to recolonizing species. Another important reason
reported by many researchers seems to be recruitment failure, either because of predation by occupying

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106 Environ. Rev. Vol. 13, 2005

species or because water chemistry conditions are unsuitable for early life stages at spawning sites that
are still affected by acid episodes.
Another main conclusion is that the fish communities that develop after liming are not thought to
be stable and species often show large swings in numbers. This is probably due to the relatively short
periods of time that these communities have had to evolve after liming. Natural, unacidified populations
generally have equilibriated to some level of “stability” after decades, if not centuries of colonization
and competition interactions. It is clearly unrealistic to assume that fish or other aquatic community
assemblages could return to pre-acidification conditions within a few years.
Other parts of lake ecosystems have also been studied after liming. Renberg and Hultberg (1992)
showed that although increases in some diatom species occurred in Swedish lakes after liming, that these
were not the species that existed before acidification. They also showed a return to previous acid-tolerant
species once liming was stopped and reacidification was allowed to proceed. Persson and Appelberg
(2001), studying the large Swedish ISELAW database, came to the conclusion that phytoplankton
biomass and numbers in limed lakes were lower than those from comparable circumneutral sites. They
also show that bacterial numbers, normalized for total organic carbon (TOC) concentrations, were also
lower at the limed sites. They ascribe part of the reduction in numbers to reduced phosphorus (P) levels
in lakes limed over a long period of time. Circumneutral lakes that do not acidify, might have a higher
nutritional status than acidified lakes in the first place, making comparisons difficult however (Persson
and Appelberg 2001). Edberg et al. (2001) showed that the number of phytoplankton species in two
treated Swedish lakes were almost doubled to 40–50 taxa after liming in 1978. They then showed a
gradual return to pre-treatment numbers when liming was stopped in one of them in 1991. Kleiven and
Lande (2000) limed a Norwegian mountain lake and found that despite higher pH and ANC levels, an
unstable phytoplankton population, as well as large variations in chlorophyll a ensued.
In Finland, Jarvinen et al. (1995) limed a high TOC lake and noted an immediate decrease in biomass
and productivity of algae and zooplankton. This was then followed by increased primary production in
deeper parts of the lake, which they ascribed to greater light availability at depth. They also noted that
the number of phytoplankton species did not change, though the species composition did change with
more cryptomonads and diatoms being present after liming. In contrast, another Finish liming study
in a slightly less organic lake (Iivonen et al. 1995) found that the number of phytoplankton species
increased, as did the composition of the periphyton.
Liming resulted in significant differences in the zooplankton Cyclops and Daphnia communities
between a limed and the reference lake in Norway (Brettum and Saloranta 2004). With only one exception
(Alona karelica), however, no acid-sensitive zooplankton species had re-established in the limed lake up
to 1999. Then in 2001, Cyclops scutifer increased in numbers and dominance while Daphnia longispina
was found in low numbers. Other changes have been found but the general impression is that re-
establishing of sensitive species will take a long time in this particular limed lake. Edberg et al. (2001)
also showed an increase in zooplankton after liming, with increases in rotifers and cladocera, probably
due to the higher primary production they measured. They also found that Bosmina sp., which is not
thought to be sensitive to acidification, decreased in numbers, probably due to a change in the competitive
environment. In another study, Walseng and Karlsen (2001) showed that the zooplankton population in
a newly limed lake in southeastern Norway, began to take on the characteristics of neutral lakes soon
after liming.
Fjellheim et al. (2001) reported that amphipod species that seemed to have disappeared from a
Norwegian alpine lake reappeared in the gut content of trout after liming. They suggested that they were
most likely never extirpated, but remained in small refugia within the lake, probably near groundwater
inputs. Improved water chemistry conditions were thought to have allowed them to expand their presence
in the lake. Iivonen et al. (1995) also showed increases in zooplankton in fish guts, showing that some
natural sampling methods are efficient at taking advantage of new opportunities. In contrast, Jarvinen et
al. (1995) showed no significant changes to zooplankton composition in a Finish lake after liming. They

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suggest that predation from resident perch populations probably had a role in controlling zooplankton,
though they did not report sampling of the fish themselves.
Study after study reports the same types of mixed results in Scandinavia (Ekstroem and Hoernstroem
1995; Edberg et al. 2001; Stenson and Svensson 1995; Svensson and Stenson 2002; Dickson et al. 1995;
Nilssen and Waervaegen 2002). Mostly, but not always, they show changes in species composition of
algae towards more diatoms. However, they do not show large changes in zooplankton populations. In
all cases, these studies show that predators already in the limed lakes take a major role in structuring
the resulting zooplankton community.
In a number of the Scandinavian studies, phosphorus (P) deficiency was identified as an important
factor in affecting plankton populations of limed lakes (Pettersson and Blomqvist 1992; Lyche-Solheim
et al. 2001; Blomqvist 2001). The loss of P, which was probably caused by a combination of precipitation
to sediments as some form of apatite (Ca5 (PO4 )3 OH) or sequestration by larger, precipitated dead biota,
seemed to limit the potential for population recovery. Blomqvist (2001) found that small additions of P
with the liming tended to assist populations to return to a more productive state.
In North America, similar types of results were being reported as in Europe. Wright et al. (1996)
showed that a shift in zooplankton species composition occurred after liming, but the new community
was not closely related to those of non-acidic lakes. Bukavekas (1993) showed that lime addition to an
acidified Adirondack lake had a significant positive effect on phytoplankton abundance and production.
He attributed the change to lower predation by zooplankton grazers that declined post-liming.
Changes in benthic invertebrates were as difficult to generalize about as was the case for plankton.
In Lake Store Howatn (Norway), the mayfly Leptophlebia vespertina population exploded after liming,
probably due to increased availability of organic matter accumulated over the acidification period, and
the slow re-establishment of other sensitive organisms (Fjellheim and Raddum 1995). Lack of recovery
of other species was attributed to the reacidification of the littoral zone area during winter and early
spring snowmelt pulses. They also felt that the long distance to potential recolonization sites with intact
populations of acid sensitive species might be important.
Persson and Appelberg (2001) found that lake benthic fauna was lower in numbers and biomass in
limed lakes than natural circumneutral ones. As already pointed out, this might also have been the result
of a generally higher nutrient status of lakes that do not acidify. Milner and Aston (1995) found an initial
depression in the benthic fauna of a limed Scottish loch, although inlet and outlet stream populations
appeared to increase. They then later measured an increase in population size of some species, despite
increased brown trout predation. Carbone et al. (1998) found that littoral benthic populations in a limed
Ontario lake, restructured from an acid-tolerant community to one more resembling neutral lakes.
However, they also felt that the lack of some expected acidophobic dragonfly species might be due to
predation by reintroduced trout.
These findings emphasize that recovery from acidification for phytoplankton and zooplankton, as
with fish, is not a simple matter of populations returning to a previous unspoiled state. Instead, not
only are populations affected by interspecific competition and prey–predator interactions, but also by
changes in nutrient supply, which must be better understood if a return to a quasi-original state is being
sought. Moreover, the process is quickly reversed when the liming effect of improved water quality is
lost.
In all European cases that reported long-term results, a cessation of liming programs led to a rapid
reacidification of waters, along with concurrent returns to pre-liming conditions. This conclusion makes
sense, but brings doubt to the rationale for undertaking liming operations that will likely be terminated
before acid deposition is at acceptable levels. It is clear from the above work that lake liming on an
operational scale must be conducted with long-term protection of lake ecosystems in mind, and that
consideration must be given to those fish species that spawn outside the lakes in streams and rivers.

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Addition of buffering materials to catchments


A number of studies have been carried out to evaluate the effect of catchment liming on surface water
chemistry. Though most of the acidity neutralization occurs in the soil of the catchment, this discussion
will only focus on the effects to drainage streams, rivers, and lakes, as soil chemistry is beyond the
scope of this review article. Olem (1991) reviewed a number of the earlier studies and most of these
produced improvements in pH, ANC, and base cations in waters draining the limed areas. A few newer
studies again confirm these results and these are reviewed here in greater detail.
One of the longest data records on water chemistry after whole-catchment liming is from Tjønnstrond,
Norway, where a 25 ha area was limed with 0–0.2 mm calcite powder in 1983 (Traaen et al. 1997).
Despite a period in 1990 when pH decreased to 5.0 and Ali increased to 70 µg L−1 , water chemistry
has been acceptable for brown trout for over 20 years since the initial treatment. They also measured Ca
concentrations increasing during pH depressions, which counteracts the negative effects of higher Ali
(Brown 1983). Reduced acid deposition and increased base saturation of the soils due to liming (Traaen
et al. 1997) have worked together to maintain and even improve the water quality again since 1990.
Based on the experience from Tjønnstrond, and realizing that damage to lichens was caused by
finely ground calcite, 80 ha of a forested catchment in southern Norway were limed in 1994 using
3 t ha−1 of 0.2–2.0 mm dolomite. Drainage stream pH increased almost immediately to 6.0 and Ali was
significantly reduced, a situation that persisted for at least 6 years after liming (Hindar et al. 2003). Using
the Model of Acidification of Groundwater in Catchments (MAGIC), Hindar et al. (2003) estimated
that the liming effect could last a further 40 to 50 years with significant increases in pH and ANC in the
drainage stream. They also included planned European sulfur emission reductions in their calculations
of the time of the effectiveness of the treatment.
Lake liming of Lake Hovvatn, which has been referred to above, was unsuccessful in protecting
eggs of lake-spawning brown trout. Much of the lake’s catchment was therefore limed using 0–2 mm
dolomite in 1999. Data from the first four winters post-liming showed a gradually increasing pH and
reduced concentration of Ali at 1, 2, and 3 m depths below ice cover of the lake receiving drainage
waters. pH was at or above 5.5 from the second year after liming, and conditions for successful egg
survival were re-established in the littoral zone of the lake (Hindar and Wright 2005). Results showed
a large increase in egg survival along with the water quality improvement (Barlaup and Kleiven 2004).
Treatment of 2 t ha−1 in another catchment (Hindar 2005) seemed to completely cancel the effects of
sea-salt-driven low pH, high Ali episodes. Stream pH values remained above 6, while Ali concentrations
remained below 20 µg L−1 during extreme weather conditions and a number of potentially toxic events
of the monitoring period of 3.5 years. Potentially toxic events were identified as periods of high relative
increase in Cl concentrations with no corresponding Na increases, indicating Na adsorption in soils.
Some collateral damage to sensitive terrestrial plants was identified in the Norwegian limed catch-
ments. The most obvious was the dieback of Sphagnum mosses in wetlands and lichens on barren rocks
when using 0–0.2 mm calcite powder (Traaen et al. 1997). Experience with the coarser 0.2–2.0 mm
dolomite grains at Hovvatn showed that the larger particles found their way from the bedrock surfaces
into the soil without harming the lichens.
The Norwegian terrestrial liming projects have recently been summarized, and the conclusion re-
garding vegetation is that whole-catchment liming using moderate doses (1–3 t ha−1 ) of coarser dolomite
on dry land causes few changes to forest vegetation. Liming-related effects on single plant species were
documented in several controlled studies, but were mainly within the natural variation expected in such
habitats (Aarrestad et al. 2004). Exceptions to this generalization seem to be related to reductions in the
fructification of mycorrhiza, the symbiotic associations between plant roots and fungi.
A catchment liming study was conducted in Wales in the late 1980s on a 0.34 km2 poorly buffered
coniferous-moorland catchment that was limed with 9 t ha−1 of CaCO3 . The wetland portions of two
other catchments were also limed using 20 and 25 t ha−1 each (Jenkins et al. 1991). Weatherley and
Ormerod (1992) found that plant, invertebrate, and fish communities partly recovered to pre-liming
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Clair and Hindar 109

conditions in drainage streams. They found that acidophilic macrophytes disappeared from drainage
streams before liming, but that the replacements predicted by their model had not yet appeared after
two years of improved conditions.
Benthic invertebrate communities of this study showed a partial return to pre-acidic conditions.
However, though the improvements to water quality were still notable 10 years after the catchment
liming, the changes in the invertebrate community were still described as modest (Bradley and Ormerod
2002). There were slight improvements in trout densities in the treatment streams, but these were also
matched by improvements in the control sites, so that the effect on this game fish was inconclusive over
the 2.5 years of follow-up study. The authors speculated that the fish communities were still influenced
by unequilibriated chemical and biological conditions. Considering the types of results reported for
lakes and streams, it is most likely that recolonization was affected by biotic factors not taken into
account by their model, such as changes in the competitive environment and the “hit or miss” nature of
recolonization.
Another aspect of this liming study was reported by Waters et al. (1991) who used different liming
strategies in two moorland catchments. They added 9 t ha−1 of limestone in a 33 ha area of one complete
catchment. In the other, they applied 16 t ha−1 only in the hydrological source area, immediately
surrounding the stream, covering 11% of the whole catchment area. Their results showed pH and Ca+2
increases, as well as Ali decreases, at both sites after liming. They also showed that it was only necessary
to lime hydrological source areas in order to improve the stream chemistry. They pointed out that this
more targetted approach was much more efficient and cost-effective in remediating stream chemistry,
compared to whole catchment liming, an approach also supported by the work of Donald and Gee
(1992). Hydrological source liming was also recommended by Miller et al. (1995) in Scotland who
found that liming the source areas of a catchment increased stream pH and Ca+2 and was especially
successful in reducing the effect of acid pulses.
Another large catchment liming project was developed around Loch Fleet in Scotland (Howells
1995). The site was underlain by poorly buffering granites, and had shallow organic, peaty soils with
moorland-type vegetation. The project proponents used between 5 and 30 t ha−1 of lime in dust, slurry, or
pellets form on a number of catchments. Their approach to deciding on dosage was based on laboratory
experiments, with an element of trial and error in the field. Their main goal was to try to provide
acceptable water chemistry for the survival of all stages of salmonids (Clymo et al. 1992). Their target
was to increase pH to 6, Ca+2 > 100 µequiv L−1 , and ANC between 10 and 50 µequiv L−1 . They did
not set a target for Ali , though they felt that improving pH and ANC would inevitably improve inorganic
Al levels.
Their liming schemes were complicated as they applied a number of treatments to various sub-
catchments draining into the loch. However, sampling the outlet stream of the loch, which integrated
results from the sub-catchment work, showed a rapid increase in pH from 4.5 to above 6 and in Ca+2
from <50 to 150 µequiv L−1 . There was a less dramatic decrease in total Al from 200 to 100 µg L−1 ,
but a significant drop in Ali from 50 to 60 µg L−1 to approximately 10 µg L−1 . All these improvements
were maintained from 1986 to 1995 when this work was last reported (Dalziel 1995).
Loch Fleet was also known to be affected by acid pulses in the streams caused by sea-salt exchanges.
Sea-salt-driven acid pulse has been well studied in the past and are known to occur in poorly buffered
maritime-influenced regions (Heath et al. 1992; Hindar et al. 1994). Dalziel et al. (1994) showed that
catchment liming caused these types of episodes to cease in the Loch Fleet study streams. The researchers
involved felt that the improvements in chemistry based on the dosages received by the catchments would
be kept up for at least another 9 years (Dalziel et al. 1994; Dalziel 1995).
Water chemistry in Loch Fleet and its inlet streams returned to a condition suitable for survival of
the various trout life stages within a few months of liming the catchments, as shown by toxicological
tests (Turnpenny et al. 1995). The lake was restocked with brown trout and these were found to be
still reproducing successfully 9 years after the liming treatment. Other parts of the biota were also

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Table 2. Summary of selected catchment liming dosages and chemical effects.

Location Reference Catchment size Dosage rate Reported effect


−1
Norway Traaen et al. 1997 25 ha 3 t ha pH from 4.5 to 7.0; improve-
CaCO3 ments lasting for at least 20
years
Norway Hindar et al. 2003 80 ha 3 t ha−1 pH increase to 6.0, Ca, Mg,
CaMg(CO3 )2 ANC also increase, Ali de-
creases; effects for at least
7 years, predict 50 year im-
provements
Wales Jenkins et al. 1991 34 ha 9 t ha−1 CaCO3 Increase pH, lasting at least
10 years
Wales Waters et al. 1991 Recharge area 16 t ha−1 CaCO3 Same effect as liming whole
catchments
Scotland Howells 1995 Various sizes 5–30 t ha−1 CaCO3 pH from 4.5 to >6.0 and
Ca+2 from 50 to 150
µequiv L−1
Germany Kreutzer 1994 2–4 t ha−1 CaCO3 5–10 years protection of
drainage waters
Sweden Fransman and Nihlgaard 20 ha 5 t ha−1 Increase pH, Ca+2 , ANC
1995 CaMg(CO3 )2
NewYork Driscoll et al. 1996; 100 and 200 ha 6.9 t ha−1 CaCO3 Gradual increase in pH,
State Blette et al. 1996 Ca+2 , ANC, probably lasting
50 years
Sudbury, Gunn et al. 2001 38 ha, metal 10.8 t ha−1 Increase pH, base cations, re-
Ontario contamination CaMg(CO3 )2 duced metals to background

followed. A number of alkalophilous periphytic diatom species returned to the loch, as were some
species never found previously (Battarbee et al. 1992; Cameron 1995). It was also recorded that algal
primary productivity doubled after liming. Researchers were not able to show long-term changes in
benthic invertebrate populations in the loch, though some of the inlet streams did show initial increases.
It was believed that the introduction of trout as predators complicated the recovery of invertebrates to
the point that no general conclusions could be drawn about that portion of the ecosystem.
A few other European studies reported effects of catchment liming (Table 2). Kreutzer (1994)
summarized German forest liming work and reported that the application of 2–4 t ha−1 of ground
limestone provided between 5 and 10 years of protection to drainage streams, depending on the soil type
and acidification level. Wilander et al. (1995) reported that a number of trial studies in Sweden provided
positive improvements of water chemistry in some sites but inconclusive results in others. Fransman
and Nihlgaard (1995) showed that dolomite applied at 5 t ha−1 in a 20 ha catchment was successful
at increasing pH, Ca+2 , and the Ca/Al ratio in receiving streams. Finally in Sweden, Dickson et al.
(1995) compared the chemistry of streams receiving water from lake and catchment liming programs
and suggested that catchment liming was a better strategy because of the slower reacidification rates
after lime applications.
There have been few relatively recent catchment studies reported in North America. Probably the
largest was done at Woods Lake in the Adirondacks region of New York State. Two 200 and 100 ha
subcatchments were limed with 6.9 t ha−1 of calcium carbonate (Driscoll et al. 1996) and results were
compared to those from lake liming that had been done previously at the same site. As with the European
studies, Driscoll et al. (1996) showed that watershed treatment caused a gradual increase of pH, ANC,
and Ca+2 and a decrease in the transport of Ali into the lake. Limestone dissolution was not shown to
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Clair and Hindar 111

be equal in all parts of the catchment, however, as drier areas did not contribute much in the way of base
cations, compared to the wetland regions treated. The slow changes to lake chemistry after catchment
liming contrasted with the rapid change that occurred after the direct lake liming (Porcella et al. 1995).
They also found that the chemistry of the littoral region of the lake was significantly improved during
episodes after catchment liming, an area which did not improve when the lake itself was limed. Modeling
of the catchment soils around Woods Lake predicted that the treatment effect might last 50 years at this
site (Blette et al. 1996).
Another study in the Adirondack region (Newton et al. 1996) also showed that liming stream catch-
ments not only increased ANC and calcium, but also provided good protection against snowmelt and
fall rain episode effects. The improvement in the inlet stream and the lake littoral area was translated
into improvement in brook trout spawning habitat and then to improved numbers of young trout in the
lake (Schofield and Keleher 1996). As with the other studies discussed previously, it was thought that
a return to pre-acidification trout population numbers was controlled by predation and other biological
factors, and not water chemistry. The authors suggested that a return to pre-acidification trout population
conditions would require a more active management approach than simply liming, such as restocking.
In Ontario, Gunn et al. (2001) limed a 38 ha catchment heavily contaminated by Cu and Ni from the
effects of a nearby smelter in Sudbury. Pre-liming annual pH values were low at approximately 4.5 and
Ca+2 values were also low (1.7–2.5 mg L−1 ). Dissolved metals were high with Cu at 56–138 µg L−1
and Ni at 320–354 µg L−1 . First, coarse dolomite (95% > 0.5 mm) was applied at approximately
11 t ha−1 . They found no decrease in acidity, a slight increase in Ca+2 , and little change in the metals
with the catchment treatment. They ascribed this result to the fact that the dolomite particles used in
dosing were too coarse to easily dissolve. They then limed 1.7 ha of wetlands (more on wetland liming
below) in the same area with 31.8 t ha−1 of a more finely ground dolomite (60% < 0.1 mm). This
greatly increased pH and base cations and reduced water metal toxicity.
Lessmark (1987) and Jenkins et al. (1991) showed that it was not necessary to lime the total catchment
to improve the quality of drainage waters. Their work showed that liming of discharge areas alone
provided the improvement in water quality needed to enhance the survival of freshwater populations.
A review of the published literature (Table 2) shows that the amounts of liming material needed in
recharge areas to make a significant and long-term difference to the water chemistry were calculated to
be between 5 t ha−1 of dolomite in southern Sweden (Fransman and Nihlgaard 1995) and 10 t ha−1 of
limestone in New York State (Brocksen et al. 1990). Obviously, the amount needed is dependent on soil
type, deposition history, and material used. However, these data show that recharge area liming does
not need to use a very large amount to achieve the set goals.
These values are compared to those used in other studies (Table 2) where whole catchment liming was
done. Generally speaking, the recommended dosages for the recharge zone liming are somewhat higher
than what was done in the whole catchment studies. However, if we assume as a first approximation that
the recharge zones are less than 1/4 the size of a typical catchment, it can be seen that this method of
increasing stream pH is much more cost effective. More work is needed to determine the best dosages
required for catchment liming, though under most conditions, based on the reports discussed above,
there seems to be no need to add more than 10 t ha−1 of limestone or dolomite to improve stream pH
and base cations.
Another approach often used in Sweden and also experimentally elsewhere is wetland liming. The
presence of wetlands is controlled by catchment characteristics as they are generally found in low-
lying areas located on or near lakes and rivers (Xenopoulos et al. 2003), or in depressions underlain by
impermeable substrates in fields and forests (National Wetlands Working Group 1988). Wetland soils
are mostly composed of slowly decomposing plant material. Their breakdown products are organic
macromolecules that contain carboxylic acid sites that contribute natural organic acids (NOA) to waters,
as well as metal complexing sites (Ritchie and Perdue 2003). The NOAs from the breakdown of plant
matter are also the basis for much of the TOC in lakes and streams. The NOAs are amphoteric at pH

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112 Environ. Rev. Vol. 13, 2005

values found in freshwaters, and thus can behave either as acids at pH levels higher than approximately
5.5 or as buffers at lower pH levels (Clair et al. 1992).
Even with no anthropogenic acidification, the pH of water draining from wetlands is naturally low.
Because they increase water acidity, and due to the good contact between runoff water and applied lime
on their surfaces, wetlands have been limed in a number of studies. Liming wetlands will change the
chemical composition of interstitial water (Kvaerner and Kraft 1995), and will increase Ca+2 and pH
to levels not normally found in the conditions that formed the wetlands.
Experimental liming of wetlands in Norway showed the same increase in pH and base cations as
shown with whole-catchment liming, though the duration of the effect was only 2–3 years as opposed to
>10 years for liming dry soils (Hindar et al. 1996). Wetland liming has not been included in operational
liming in Norway, as massive die-back of Sphagnum mosses often occur.
In Sweden wetland liming has been a significant part of the operational liming program, with about
1500 sites treated in the period 1985–1993 (Wilander et al. 1995). As with Norway, wetland liming has
effectively increased water pH and base cations, and the duration of the treatment has been relatively
short compared to dry land liming (Borg et al. 1995). Also as in Norway, wetland liming has caused rapid
and major changes in wetland vegetation. Larsson (1995) reports major losses of Sphagnum mosses and
liverwort (Hepaticae) vegetation in various studies. It was also realized in Sweden that natural wetlands
were being limed to pH values higher than existed pre-acidification values. This caused a re-evaluation
of the Swedish approach to wetland liming, which then took a more sophisticated approach in site
selection (Warfvinge et al. 1995).
Catchment liming in Loch Fleet showed a number of moss species thriving or unaffected, while
two acidophilic mosses, Sphagnum capillifolium and S. papillosum, were completely eradicated where
they came in contact with limed conditions (Clymo et al. 1992; Bragg and Clymo 1995). Wilkinson
and Ormerod (1994) found that another moss species, Nardia compressa, was also greatly reduced in
coverage after liming in Wales, and that no other species had moved in to replace it 5 years later. Gunn
et al. (2001) arrived at similar conclusions in the Sudbury, Ontario region. They limed 15 wetlands with
fine particled dolomite and showed adverse effects on wetland plant communities, at the same time as
showing increases in pH.
The practice of liming brown water source areas in Sweden was questioned by Bishop (1997)
and Jansson et al. (1992) who felt that naturally acidic waters and their biological communities were
being disturbed by liming. Laudon and Hemond (2002) showed that organic acids were often the major
source of acidity in northern Sweden, though anthropogenic acidification contributed significantly to
low pH and the fish problems only during snowmelt. It was felt that the best method of avoiding
needless alterations to natural communities was to develop and use models (Laudon et al. 2001, 2005)
or parameters (see also Lydersen et al. 2004) to better identify anthropogenic acidification before any
decisions are made regarding liming.
An issue that arises in catchment liming is due to the fact that microbial processing of organic
matter is higher in less acid soils. This eventually results in greater breakdown of soil organic material
and increased leaching of NO3 − (Brahmer 1994; Meiwes 1995). Lundstroem et al. (2003) not only
found increased nitrification and thus higher NO3 − in soil solutions of limed catchments, but also found
changes in the soil mycorrhizal fungi community. Durka et al. (1994), however, showed that acidified
forests had lost their ability to properly process NO3 − and that liming forest soils probably allowed
them to return to a more “normal” state, which involved greater N release from better conditioned soils.
This topic is currently undergoing a great deal of research by soil scientists and is beyond the primary
focus of this review and these authors’ expertise. Nevertheless, we studied the literature to see if N
cycling in water was affected by catchment liming.
The aquatic literature shows that increases in soil NO3 − does not necessarily lead to chemically
significant increases in stream nitrate. Hultberg et al. (1995) found no NO3 − and NH4 + changes in runoff
from limed Swedish catchments. Driscoll et al. (1996) measured some increases in soil and stream water
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Clair and Hindar 113

NO3 − , but not enough to affect stream ANC. Hindar et al. (2003) showed no significant increase in
stream NO3 − after liming a Norwegian catchment. On the other hand, Traaen et al. (1997) and Hindar
(2005) show significantly increased NO3 − in three other streams where the catchments have been limed.
Van Hees et al. (2003) also show NO3 − increases in flows from limed sites located in southern Sweden.
Based on these studies, we suggest that liming of catchments may increase NO3 − in drainage waters,
although this is not always the case. Most of the studies described above show that catchment liming
can improve water chemistry conditions in two ways. First, it can improve the chemistry of baseflow
waters. Liming improves surface soil and interstitial water chemistry that eventually is translated into
improved baseflow (higher pH, calcium, and lower Ali ) from the catchment into drainage streams.
Secondly, liming is seen to improve water chemistry during high runoff events that often bring acid
pulses. The main water pathway for acid pulses is through the surface soil layers (Mulder et al. 1991)
where most of the liming material is deposited and where it remains for a long period of time. Acidic
waters thus come in contact with buffering materials during episodes and thus tend to be neutralized,
with a concurrent release of calcium and magnesium to the stream water and retention of Ali in the soil.
Experimental and operational liming in Sweden show that terrestrial liming only needs to be done in
water source areas, and not over the whole catchment to help improve water chemistry. Results in Wales,
Scotland, and Norway suggest that only liming source areas is as successful as whole catchment liming,
although the duration of the effect may be shorter. Damage to vegetation will also be more serious in
these areas, both due to dominance of sensitive Sphagnum mosses in wet areas and to the higher area
doses that might be needed. The cost-effectiveness of source area versus whole catchment can only
be compared on the basis of the total length of the liming period, i.e., until re-liming is necessary for
maintaining good water quality for sensitive organisms. Catchment liming was not successful where
the size of lime or dolomite particles was too large to provide rapid dissolution, or where the amount
used was insufficient (Gunn et al. 2001).

Special issues in liming


The effect of liming on dissolved organic matter in water
There seems to be no consistent findings from research studies regarding the influence of catchment
liming on the generation of TOC in drainage waters (Table 3). Driscoll et al. (1996) report higher TOC
levels in Woods Lake and inlet streams after catchment liming. Grieve (1990b) also shows increased TOC
exports in the stream around Loch Fleet. On the other hand, Edberg et al. (2001) show no TOC differences
between limed and reacidifying catchments in Sweden. Hindar et al. (2003) found a significant increase
in TOC in a moderately coloured stream, whereas Hindar (2005) recorded a significant decrease and
no change, respectively, in two other moderately coloured streams after whole-catchment liming with
dolomite.
The effect of whole lake liming on TOC is also complex. Wright et al. (1996) show a short-term
increase in water clarity (which is partly caused by lower TOC) in a Minnesota lake, with recovery to
pre-liming conditions within a few months. Persson and Appelberg (2001) show no differences between
TOC of limed and unlimed lakes in the Swedish national program. Simmons et al. (1996) report no
differences in TOC before and after liming a stream watercourse in Massachussetts. To confuse matters
further, Wilander et al. (1995) report that the general tendency in Swedish lakes is that high colour (i.e.,
high DOC) waters become lighter after liming, while lower colour waters either increase or decrease.
The reasons for the different types of results most likely have to do with a combination of processes
in the catchments and lakes, as well as climatic variables. Brooks et al. (1999) show that acid forest
soils leach out less TOC than better buffered ones. Lundstroem et al. (2003) and Karlik (1995) also
show that limed soils (which include wetlands) have higher organic matter decomposition rates than
more acid soils. This causes more organic macromolecules to be broken off soil organic matter and
released to interstitial waters and then to runoff. This might explain why streams and lakes containing

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114 Environ. Rev. Vol. 13, 2005

Table 3. Total organic carbon concentration direction changes after liming for the studies reviewed.

Author Region Liming type Lake Stream


Grieve 1990b Scotland Catchment Increase
Driscoll et al. 1996 Adirondacks Catchment Increase Increase
Edberg et al. 2001 Sweden Catchment No change
Hindar et al. 2003 South Norway Catchment Increase
Hindar (2005) South Norway Catchment Decrease and
no change
Wilander et al. 1995 South Sweden (high colour) Lake Decrease
Wilander et al. 1995 South Sweden (low colour) Lake No change
Simmons et al. 1996 Massachussetts Stream No change
Wright et al. 1996 Minnesota Lake Decrease*
Persson and Appelberg 2001 South Sweden Lake No change
* Short-term change only.

limed catchments often have more TOC entering them. Small lakes and streams without wetlands or
organic soils in catchments are less likely to receive more organic matter and thus cause the situation
reported by Wilander et al. (1995) of a mixed bag of trends. A previous review (Porcella et al. 1990)
reported that highly organic waters did not require special evaluation for treatment with limestone, as
the potential changes were generally benign from an environmental point of view.
Other factors may come into play with TOC conditions. The liming of lakes and streams (as opposed
to catchments) tends to increase primary production that, in this case, seems not to have an effect on
overall TOC. It may be that allochthonous TOC is converted to an autochthonous form by microbial–algal
interactions. However, this type of change would only be detected using more sophisticated approaches
than reported in the published literature we found. In temperate regions, TOC production is driven in
large part by precipitation through wetlands (Schiff et al. 1998). The more water runs through wetlands
and soils, the more TOC is generated in the receiving water bodies, so that changes measured in the
above papers may be caused by factors other than liming. The studies reviewed here have not attempted
to get at the heart of this matter, most likely because TOC is not a targetted outcome of liming, but is
more of a side result of the process.

The effect of liming on dissolved aquatic aluminum and other metals


One of the main effects of acid precipitation is that strong acid anions are partly balanced with
Ali and other metals in soil water (Reuss et al. 1987), from where they eventually find their way into
water courses. The more acidified the soil, the more Ali will be released. Al chemistry in freshwaters is
complex (Stumm and Morgan 1996), but, as a rule, the lower the pH of a freshwater solution, the more
likely the Al is to be in the toxic inorganic form (Leivestad et al. 1987). At pH 4–4.5, most of the Al will
be in the Al+3 form. At intermediate pH levels (5.0–6.0), Al is still positively charged, but mainly as
Al(OH)+2 and Al(OH)2 + at typical natural water temperatures. All these positively charged ion species
are termed Ali (inorganic monomeric Al) in this paper. At pH 6–7 Al may be precipitated as amorphous
Al-metal-organic complexes that are non-toxic and do not cause fish mortality.
Ali toxicity to fish in acidified waters was discovered in the late 1970s (Cronan and Schofield 1979;
Dickson 1978), and has been extensively studied since then. Al accumulates on fish gills that affects
blood chemistry and impairs physiological processes (Muniz and Leivestad 1980 and e.g., Kroglund
and Finstad 2003). Ca ameliorates the toxic effect of Ali (Brown 1983). Some studies have shown that
TOC will reduce, if not completely neutralize Ali effects (e.g., Roy and Campbell 1997), as it complexes
with Ali , making the metal unavailable for adsorption onto fish gills. Studies have also shown that Ali
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Clair and Hindar 115

detoxification is relatively rapid, as impaired fish exposed to higher pH and thus lower Ali concentrations
recover within hours of being placed in higher pH environments (e.g., Kroglund et al. 2001).
Other metals are also released by the acidification of soils, but as Al is one of the most common
elements on the surface of the earth, and as it has the most obvious effects on the health of aquatic
organisms, most of the acidification literature has focussed on it. A number of studies have tracked
Ali concentrations in drainage waters after catchment liming. Immediately after liming of Loch Fleet
catchments, dissolved Ali concentrations were reduced by up to 80% (Grieve 1990a). Turnpenny et al.
(1995) later reported that 8 years after catchment liming, Ali was still at non-toxic levels. In Wales,
Waters et al. (1991) also showed decreasing Al concentrations in streams draining limed catchments.
At the Gjerstad experimental area in Norway, Hindar et al. (2003) applied dolomite at 3 t ha−1 . After
the treatment, less Al was released to the drainage stream of the limed catchment, as Ca and Mg were
being exported to compensate. The results of post-liming monitoring of 10 trace metals in the streams
also showed decreases in dissolved metals at the limed sites. Reductions in Ali were also achieved
at the Norwegian west coast after the application of 2 t ha−1 of dolomite in the Suldal catchment in
1999. Three and a half years after treatment, there was still almost no post-liming mobilization of Ali
during sea-salt episodes (Hindar 2005), a remarkable result for a hilly landscape receiving 2.5–3 m
of precipitation each year. In North America, Driscoll et al. (1996) also found that watershed liming
decreased Al exports from catchments to drainage streams and lakes.
The direct liming of lake or stream waters provided similar results to catchment liming in terms of
changes in Al toxicity. Andrén et al. (2001) compared stream Al concentrations in limed and unlimed
acidified Swedish streams and found Ali levels to be significantly lower in the limed streams. Borg et al.
(2001) summarized results from large-scale Swedish surveys and also found that liming significantly
lowered dissolved Al, Cd, Fe, Mn, and Zn in lake and stream waters. Booth et al. (1993) found that
liming interstitial shoals in Ontario lakes reduced Ali in spawning beds. Menendez et al. (1996) also
showed Ali concentrations to be reduced downstream of a lime doser operation.
Egeberg and Hakedal (1998) studied the sediments of a lake located downstream of a limed river in
Norway. They found that lake sediments that were deposited after liming contained higher Cd and Zn
concentrations, which they assumed were scavenged by Fe-enriched acid insoluble particles at higher
pH values. After the liming treatment was stopped, Wallstedt and Borg (2003) found a remobilization of
metals from sediments into the water column, showing that sediment metal precipitation was a reversible
process.
There was a concern raised in the literature about severe toxicity caused by unstable Al-chemistry
when Al-rich waters mix with higher pH water. This mixing caused rapid polymerization of Al into
complex hydroxylated forms that precipitate on fish gills (Rosseland et al. 1992). Weatherley et al.
(1991) found that Al precipitated and caused mortality to caged salmon in mixing zones within 30 m
of liming sites. However, this problem was no longer evident within 100 m, as caged fish had a 100%
survival rate when slightly removed from the liming operation. Åtland and Barlaup (1995) studied this
problem and concluded that, in field situations, salmon seemed to be able to avoid these potentially
dangerous situations.
Summarizing the issue of metals, especially Al, and liming, all research is unequivocal in showing
that liming catchments reduces the amount of Al exported from soils into streams. This is likely due to
changes in soil chemistry (increased base saturation) and thus to base cations replacing Al as positively
charged ions in export waters. Studies also show that, as expected by theory, Al becomes less toxic at
higher pH values because of a change in Al ionic speciation that occurs at higher pH, or through co-
precipitation with dissolved organic matter. The potential for the rapid polymerization of Al immediately
below liming operations has been shown to exist. However, the research reported has shown that this
is not as serious a concern as fish seem to be able to avoid zones dangerous to them. Moreover, the
long-term effects of reducing acidity and Al toxicity are much more important for the well-being of a
population than a very local problem of Al hydroxylation and precipitation.

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Discussion
Based on our analysis of the literature, we must come to the conclusion that with very few exceptions,
the use of lime or dolomite on either catchments or water bodies is not deleterious to aquatic ecosystems
either in the short or long term. The one exception to these conclusions is the liming of wetlands. Many
of the wetlands located in regions affected by acid rain are naturally acidic, and the addition of base
cations to their soils leads to novel conditions that can cause drastic changes to the flora, especially
acidophilic mosses.
Most of the studies we report on have been able to modify the chemistry of receiving waters
to a desired state. Generally, the biological communities in rivers and lakes that have been limed
tend to accumulate more acid-sensitive species, and have not shown any obvious further degradation
in community composition or structure. However, returns to what may have been pre-acidification
ecological conditions have been more elusive. An important reason for this is that the chemical changes
brought about to streams, lakes, and catchments are usually temporary, as reacidification is bound to
return ecosystems to their previous “damaged” state upon cessation of the liming effort. The reversion
is immediate when liming streams and rivers, usually within a few years when liming lakes, and
between 10 and 50 years when liming catchments. So the question that must be asked is whether
liming is a worthwhile exercise in the long term. As we show that liming is not generally harmful to
the environment, deciding whether or not to lime will involve a number of social, policy, and even
philosophical considerations.
There have been compelling arguments made against liming to mitigate acid rain effects. The first
one is partly philosophical, partly pragmatic and was best stated by Schindler (1997). In short, this
argument states pollution prevention is the best mitigation strategy, and that liming masks the fact that
ecosystems are being seriously damaged by human activity. This argument is supported by the work of
Gee (2001) who analyzed the mitigation needs of Wales, a relatively small and highly populated region,
compared to Scandinavia and much of acidified North America. Gee (2001) used an evaluation matrix
approach that took into account the expert opinions of scientists, environmental managers, and political
advisors to rank the desirability of mitigation options for improving water chemistry of acidified Welsh
streams and lakes. Of the 11 options that were considered, S and N pollution reduction (options 1, 2,
and 4) were ranked highest, followed by improvements in forestry practices to reduce conifer-driven
soil acidification (option 3). The direct liming of streams came 5th on the list, while source area liming
was 8th.
On the other hand, Howells and Brown (1992) supported the need for some mitigation efforts. They
argued that the time needed to reverse the long-term cumulative impact of acidification was too long in
certain regions to simply let nature recover by itself with the agreed-to emission reductions. They argued
that irreversible, negative changes might occur to some aquatic populations without some temporary
intervention. One application of this argument is that focussed liming can help avoid the extirpation of
populations with unique genetic characteristics, such as the Aurora trout in northern Ontario (Snucins
et al. 1995). Another example are the Atlantic salmon populations in the southern and eastern shores
of Nova Scotia. They have developed genetic modifications, which allow them to tolerate low ionic
strength, high organic acidity conditions. Populations are already extinct in a number of rivers (Watt
et al. 2000) and are on the brink in others. It is thus important to protect some populations carrying
these traits, so that recolonization by adapted fish can reoccur when acidification effects in this region
are finally reversed by pollution reduction efforts predicted to occur, in five or six decades (Clair et al.
2004).
To some extent, Schindler’s (1997) objection and Gee’s (2001) analysis have been overtaken by
events. New Canadian Federal – Provincial agreements, and the European Gothenburg Protocol, have
mandated emission cuts that will be roughly 75% below early 1980 levels by the year 2020. A number
of legislative options are also currently debated in the United States that may achieve similar goals.

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Pragmatically, it could be argued that acid pollution reduction is occurring as rapidly as can be realis-
tically achieved in both Europe and North America. If these reductions do come into place in the next
decade, then it could be assumed that Schindler’s and Gee’s greatest concerns are now being addressed.
Despite some optimism on the pollution reduction front, recent dynamic acidification modeling in
Europe and North America (Larssen et al. 2003; Clair et al. 2004) confirms that even with aggressive
emission cuts in Europe and North America, large numbers of lakes and rivers in sensitive regions
will not recover to pH and ANC levels suitable for sustaining healthy aquatic communities for decades
after emission reductions, because of base cation depletion from catchment soils. Schindler (1997) also
makes the case that ecosystem modifications by humans rarely achieve the desired goals, but usually
bring up other, unexpected and sometimes undesirable problems. This review shows that this seems to
be the case when liming wetlands.
The main shortcoming of liming programs is that ecosystems do not completely return to pre-
acidification conditions for several reasons. First, unstable or inadequate chemistry conditions may
occur when using unsuitable liming strategies. Secondly, species interactions and a lack of sources for
sensitive species reintroduction will affect community composition. Generally, the papers quoted in this
review show that targetted fish species usually, but not always, can be assisted in returning to viable
numbers, as long as pH and ANC (and thus lower Ali ) can be maintained over long periods of time and
that restocking or protection against predators is done. More often than not, however, the rest of the
ecosystem is never completely returned to pre-acidification conditions and the new communities may
be relatively unstable and prone to large changes in composition.
Based on the results described above, one can conclude that liming strategies may be devised to
achieve limited objectives for most lake and running water situations. However, we also identify short-
comings and side effects of some of the techniques. A most important point when trying to recover fish
populations is that other management tools might be needed to assure the return of targetted species
(e.g., Alenäs et al. 1991). As several authors have emphasized, biological aims should control the liming
approaches to be selected. Moreover, it is important that liming influence the life stage most sensitive
to acidification.
To understand why liming is often considered to mitigate acidified ecosystems, it is important to
understand what organisations want to lime and why they want to do so. Both these authors have realized
that there is a great desire amongst non-governmental environmental organizations (NGOs), especially
fishing enthusiasts, to protect or accelerate recovery of valued ecosystems (e.g., Hindar 2001). It is
quite difficult for governments to tell taxpayers to do nothing and wait for nature to respond on its own,
especially if the wait will take decades.
A good example of public policy driving the need to act occurred in Scandinavia in the early 1980s.
Public awareness and political concern for loss of biodiversity and reduced possibilities of recreational
fishing resulted in the development of public funding programs in Norway and Sweden that are still
ongoing 20 years later. Fishing organizations, landowners, and municipalities are the main applicants
for funding. Liming practices are supervised by federal government agencies in cooperation with local
environmental authorities (Sandoy and Romundstad 1995). The Norwegian government is also more
directly involved in ongoing liming of 21 important salmon rivers (as of 2004). Other lakes and streams
are limed as part of the ongoing research and development (R&D) program under research contracts.
There have been a number of attempts in the past, to help guide the desirability and potential
success of liming projects. One of the earlier ones was by Sverdrup (1985) who developed a flow-
chart approach for the planning of liming efforts that also included a cost-efficiency evaluation. Another
attempt at rationalizing the liming decision-making process was done in the Adirondack region by Gloss
et al. (1989) who focussed their work on managing brook trout populations. They mostly emphasized
the practical aspects of liming to allow trout fishing such as legal issues of access to lakes and streams,
restocking approaches, and suitable genetic stock. They also discussed the setting of suitable water
chemistry and population targets for the recovery of that species. Apart from these two approaches, we

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discovered no comprehensive published procedures for assessing liming needs, as most of the procedures
and rationales of the studies we describe were determined in a relatively ad hoc fashion.
The precedent set in Scandinavia as well as the combination of scientific and public interests leads
to our view that pressure to conduct liming will occur elsewhere in Europe and North America in the
future. If new liming projects are to happen, however, it will be important to ensure that proponents and
regulators follow a clear process to ensure that they do not further damage ecosystems and that they have
a reasonable chance of meeting their objectives. In order to help in achieving these two conditions, we
list a number of issues that need to be addressed before a liming project receives serious consideration.

(a) First, there needs to be a good rationale to justify attempting to modify an ecosystem, and the
parts of the ecosystem in need of protection need to be clearly identified. It is important to insure
that even if a fish species is clearly in need of protection, other parts of the ecosystem (e.g.,
prey, predators and other competitors, access to habitat, other types of pollution effects) will not
provide another obstacle to population recovery. Neglecting this step can only lead to the failure
of a project.

(b) There must be clear understanding of the target species life cycle. If a fish species is to be recovered
or protected, are all the vulnerable life stages protected? For example, there is no point improving
a species’ passage by liming a stream if the conditions at the spawning grounds are not allowing
successful hatching to occur.

(c) The proponents must have reasonable expectations of what is achievable with the methods they
will be using. As the Norwegian experience shows, in order to get a successful program on a large
river system, there is often a need for more than one doser. Half measures are usually a waste of
time in this kind of work.

(d) The proponents must have a good understanding of the time to recovery of the system. Dynamic
acidification modeling reveals that water chemistry recovery may take decades in certain areas
with poor soils, such as southern Norway or Nova Scotia. There is no point beginning a liming
program if proponents are only able to carry it out for a few years. This is clearly one of the major
advantages to catchment liming as its effects can last for decades instead of hours in the case of
in-stream dosing.

As Gee’s (2001) analysis also points out, there are a number of other uncertainties associated with
mitigation that we have not discussed. Factors such as climate change with more extreme weather and
reforestation can modify hydrological and pedological cycles in ways that might offset gains made
by liming. These types of pre-project assessments need to be done as a first step in deciding on the
suitability and desirability of mitigation approaches and will provide different results based on local
conditions.
In our review, we have consciously refrained from discussing financial costs of the various liming
options, as these will vary based on the region, water body size, availability of neutralizing agents, and
changes in technology. Analysis of benefits to ecosystems and society versus costs is clearly warranted
when expensive operations are needed to achieve a target. For example, a recent analysis based on
measurable income in the Mandal River (Norway) region shows an increase in local added value of
three times the cost of liming with around 6000 t of calcite each year (Mauland 2004) attributable to
increased visits of outside anglers. This type of result is not necessarily guaranteed in all liming projects,
however. Moreover, certain situations such as protection of endangered species are not conducive to
this type of cost-benefit analysis.
In the final analysis, ecosystem liming must be viewed as a tool to keep ecosystems or targetted fish
populations from being irretrievably lost until nature can restore itself under less polluted conditions.
It cannot be a substitute for pollution prevention, nor should it be used to create conditions that did not

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Clair and Hindar 119

exist before the acidification problem existed. An important issue with liming is that it will likely need
to be done over a long period of time in highly acidified systems, as reacidification will occur once the
effect is allowed to lapse. If this happens, any “positive” change in populations will be reversed, thus
making the whole previous exercise a waste of time and money.

Summary
Our review shows that liming programs can be designed to improve water chemistry conditions of
streams, rivers, and lakes. When properly designed and consistently managed, a combination of liming
and stocking programs will allow the recovery of targetted fish species in formerly acidified waters.
However, research also shows that ecological recovery is not a straightforward process. Factors such as
the presence of acid tolerant predators and availability of recolonizing species will affect the rate and
direction of recovery.
We also show that for many parts of Europe and North America, the recovery of soil and thus
drainage waters from the effects of acidification will take decades to occur or not occur at all with
planned emission reductions. This means that in heavily affected areas, recovery of water chemistry and
thus of aquatic ecosystems will take decades even under the most optimistic acid reduction scenarios.
Such scenarios demand a long-term strategy for improving the ecological status in affected areas. We
conclude that liming may be part of this strategy. Terrestrial liming has the broadest potential as it
supplies the soil with base cations, thus counteracting the leaching of acid and toxic ions at the source.
As any liming project considered in highly acidified regions will have to be undertaken for a long time,
terrestrial liming provides the simplest way of achieving that goal.
In effect, though, the ultimate goal of mitigation is the recovery of ecosystems to a “natural” state,
and this can only be achieved through the cessation of acidification effects and the passage of time
to allow soils and aquatic communities to recover. The real objective of any new mitigation program
must be to keep further damage from occurring until the effects of pollution controls are reflected in
catchment soils and therefore by drainage waters.

Acknowledgements
This review was started because of a request from the Nova Scotia Atlantic Salmon Federation
to advise them on strategies to recover local Atlantic salmon populations. In particular, Lewis Hinks
their Executive Director was a great help and encouragement. We also thank Dr. Richard Wright of
the Norwegian Institute for Water Research (NIVA) who reviewed this work. No study of this type
occurs without the help of good librarians. Jean Sealy of Environment Canada, Sackville and Berit
Kramer at NIVA were instrumental in getting us hard-to-reach documentation. This work was funded
by Environment Canada’s Acid Rain Program and by the National Research Council in Norway.

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