Dendrochronologia 29 (2011) 31–40

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Dendrochronologia
journal homepage: www.elsevier.de/dendro

Reconstructing contamination events on riverbanks in southern Québec using

dendrochronology and dendrochemical methods
Diane Saint-Laurent a,∗ , Patricia Duplessis b , Julien St-Laurent c , Luc Lavoie d
a
UQTR, Géographie et Laboratoire de recherche en géomorphologie fluviale, C.P. 500, Trois-Rivières, QC, Canada G9A 5H7
b
Environnement Canada, 1141, route de l’Église, C.P. 10100, Québec, QC, Canada GIV 4H5
c
Direction Environnement et Développement durable, Ville de Trois-Rivières, C.P. 368, Trois-Rivières, QC, Canada G9A 5H3
d
Group GDG Environment, 430, rue Saint-Laurent, Trois-Rivières, QC, Canada G8T 6H3

a r t i c l e i n f o a b s t r a c t

Keywords: The riverbanks of the Saint-François and Massawippi Rivers are affected by hydrocarbons and heavy
Dendrochronology metals to varying degrees. The events associated with this riverbank contamination are not documented
Dendrochemistry in the government reports or archives, which is why dendrochemical methods are useful for dating such
Red ash
pollution events. Samples of alluvial soils and trees were taken from the banks of the Saint-François River
Contaminated soils
in Windsor and Richmond as well as the Massawippi River, where the level of hydrocarbon (C10 –C50 )
Hydrocarbons
Floods contamination in the banks is low to moderate (300–700 mg/kg of dry soil). Core samples were taken
from seven red ash (Fraxinus pennsylvanica Marsh.) and dendrochemical analyses were done on the tree
rings. Dendrochemistry was successfully used to determine that there were heavy metals in the rings,
and also to estimate the date of the contamination events by using tree-ring wood. Several contamination
events were identified through the presence of lead and other contaminants in the xylem of the trees
analyzed at the selected sites. This suggests that various contaminants were transported by the river on
several occasions and deposited on floodplains during successive floods. Also, a marked increase of some
heavy metals like aluminum and nickel in the tree specimens can be attributed to recent atmospheric
pollution. The emissions of metal-bearing particles may have varied widely over the century due to the
different types of industrial activities, technological changes and atmospheric emission regulations. All of
these anthropogenic changes reflected in the rings of the trees that showed variations in the geochemical
profiles. Though several major contamination events can be determined, it is still difficult to identify all
of the potential sources of pollution, of which there are many in this vast catchment.
© 2010 Istituto Italiano di Dendrocronologia. Published by Elsevier GmbH. All rights reserved.

Introduction Vroblesky, 1995; Watmough, 1999; Yanosky et al., 2001; Padilla

Several sources of contamination currently found in the envi-
ronment are a legacy of past industrial activity. Mining and
industrial activities in many cases resulted in the major pollution
and contamination problems now found in numerous environ-
mental media (e.g. soil, sediment, water, biota). Mining, the use
of numerous chemicals, and increased used of petroleum prod-
ucts in various forms were added to other environmental pollution
sources, which can be easily traced in rivers and lakes (Christensen
et al., 1996; Malawska and Wilkomirski, 2000; Dror et al., 2001;
Ferretti et al., 2002; Nikanorov and Stradomskaya, 2003). Vari-
ous researchers have been working on detecting the contaminants
contained in soils, sediments and aquifers through the use of
dendrochronological and dendrochemical methods (Yanosky and
∗ Corresponding author. Tel.: +1 8193765011x3674; fax: +1 8193765179.
E-mail address: diane.saint-laurent@uqtr.ca (D. Saint-Laurent).
and Anderson, 2002; Smith et al., 2008). In these studies growth
rings can serve as indicators of environmental contamination
events affecting aquifers and soils. Many studies also deal with
cases of contamination by heavy metals detected in the growth
rings (Baes and McLaughlin, 1984; Guyette et al., 1991; Hagemeyer,
1995; Malawska and Wilkomirski, 2000; Bindler et al., 2004). Vari-
ous factors may indeed influence the concentration of heavy metals
in the wood of trees, including the phenomenon of radial translo-
cation (Yanosky and Vroblesky, 1995; Yanosky et al., 2001; Meerts,
2002), the bioavailability of metals and ion mobility in soils (Padilla
and Anderson, 2002; Kabata-Pendias, 2004), as well as edaphic and
climatic conditions (McLaughlin et al., 2002; Padilla and Anderson,
2002; Savard et al., 2006).
Contamination events can be also detected either by a decrease
in the growth of the tree (observable through a decrease in the
width of the annual rings) or by an increase in the interannual
variation of the growth ring (Baes and McLaughlin, 1984; Jordan
et al., 1990; Watmough, 1999; Balouet and Oudijk, 2006). A high

1125-7865/$ – see front matter © 2010 Istituto Italiano di Dendrocronologia. Published by Elsevier GmbH. All rights reserved.
doi:10.1016/j.dendro.2010.08.005
32 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40
level of contaminants in the soil is generally required for significant
changes in the reduction of growth rings to be seen (Hagemeyer,
1993; Kabata-Pendias, 2004). The absorption of soil contaminants
from the roots to the cambium may span one growth year or more
(Donnelly et al., 1990), which could create a time lag between the
year of contamination and when the latter was recorded in the tree,
which is why it is important to use more than one tree at a contam-
ination site. The possible time lag may depend on several factors,
including the availability of the metal, the physiological charac-
teristics of the species, the tree response (phytotoxicity), the age
of the specimens, and soil conditions (Cutter and Guyette, 1993;
Smith and Shortle, 1996; Ferretti et al., 2002; Smith et al., 2008).
In some cases, very high concentrations of metal elements in the
soil may not be “detected in the wood of fast-growing” (Smith and
Shortle, 1996). Mention is also made of problems related to the
tree’s response time, which can vary depending on the species and
the radial translocation process (DeWalle et al., 1991; Hagemeyer,
1995; Smith and Shortle, 1996; Bindler et al., 2004).
More recently, some studies have reconstructed the contam-
ination events by analyzing the chemical composition of the tree
rings by integrating soil chemistry, isotopic composition and atmo-
spheric parameters (Tarhule and Leavitt, 2004; Anderson et al.,
2005; Savard et al., 2006). These researchers used a combination of
natural (Ca, Ca/Mn, ␦13 C) and anthropogenic (Cd, Pb, 206 Pb/207 Pb,
208 Pb/206 Pb) geochemical tracers which allowed the detection of
successive of atmospheric, pedological and edaphic changes related
to high-salinity sites, air pollution and industrial activities in the
mining area.
This study deals with identifying and analyzing the contami-
nants found in the growth rings of trees using dendrochemistry
methods. The species selected for the study is red ash (Fraxinus
pennsylvanica Marsh.), found in flood-prone areas along the banks
of the Saint-François and Massawippi Rivers (southern Québec).
Based on our prior work, we were able to identify various types
of contaminants along the banks of these rivers (e.g. hydrocar-
bons, heavy metals) and to draw up their spatial distribution in
alluvial plains (Saint-Laurent et al., 2008a,b). In addition to the
heavy metals contained in alluvial soils, we were easily able to
identify at the base of the soil profiles hydrocarbon-contaminated
(C10 –C50 ) layers extending over more than 100 km of riverbank
between the former mining site (Eustis mine) and the municipality
of Drummondville (Fig. 1). The source of the contamination (hydro-
carbons) appeared to be at Eustis mine that had been closed since
1939. The hydrocarbon-contaminated layers are easily visible in
the riverbanks along the Massawippi River with a dark colouring
and also a marked odour. These hydrocarbon-contaminated lay-
ers may originate from one or even several accidental spills or
intentional discharges from the former Eustis mining site. The use
of lead in petroleum products (e.g. gasoline, heating oil) before
1990 and the fact that it was no longer used after this date (see
CEPA, 1990) seems a good indicator in this study for the identifi-
cation of hydrocarbon contamination in the riverbanks, as well as
for estimating the date of the contamination events through the
use of tree-ring wood. Other heavy metals (e.g. Al, As, Cd, Cu, Ni,
Zn) are also analyzed in the growth rings in order to detect and
date other contamination events that may have occurred along the
Saint-François and Massawippi Rivers.
Materials and methods
Regional setting
The sites studied are located along the Saint-François and
Massawippi Rivers, which are part of the Saint-François River
catchment (southern Québec). The two rivers flow through agri-
cultural and urban areas and also cross former industrial and
mining sites, including the Eustis-Capelton mining complex found
along the Massawippi River. Because of past industrial and min-
ing activity, numerous government reports were produced on the
quality of the water in these rivers and talk about the degrada-
tion and contamination of these waterways and their toxic effects
on aquatic wildlife (Berryman et al., 1996, 2003). The reports
state that the waters of the Saint-François and Massawippi Rivers
were severely contaminated by mining, industrial and agricul-
tural waste (e.g. mines, pulp and paper industries, chemical and
textile manufacturers). The products released by these industries
and manufacturers in the rivers contain heavy metals, polycyclic
aromatic hydrocarbons (PAH), volatile organic compounds, total
suspended solids (TSS), phosphorus, inorganic compounds, traces
of PCBs and other contaminants (MEF, 1996; Berryman et al.,
2003; Painchaud, 2007). The ancient mining sites (Eustis, Capel-
ton) located along the Massawippi River are also major sources
of pollutant discharge in watercourses in this area (Ross, 1975).
The government reports (Berryman et al., 1996, 2003) showed that
these mines were responsible for heavy metals and copper concen-
trations detectable in the Massawippi and Saint-François Rivers as
far as Bromptonville.
In the various government reports that were reviewed, no
mention is made of riverbank contamination or floodplain soil
contaminated. Archival documents and regional newspapers were
reviewed to find information that could lead to the determination
of the probable source of contamination and explain the events that
could account for the presence of contaminated soils (e.g. presence
of hydrocarbons layer) in the banks of the Saint-François and Mas-
sawippi Rivers. Two articles referring to cases of water pollution (oil
discharge) in the Saint-François River were found in local newspa-
pers. They appear to have occurred in October 1955 and May 1963,
but none of the articles indicated the source of the contamination
or the events that may have caused it. However, neither article
mentions that the Massawippi River was affected by the same pol-
lution events, even though we found hydrocarbon contaminated
soils along the Massawippi River.
Analysis of contaminants in the riverbanks
Following the analysis of the spatial distribution of the contam-
inants (see Lavoie et al., 2006; Saint-Laurent et al., 2008a), three
sites were selected (Richmond, Windsor and Massawippi sites),
which are among the sites most affected by the contamination.
These sites are located directly on the riverbanks between the
municipalities of Eustis and Drummondville (Fig. 1). For each
site, a trench was dug along the riverbank in order to reach
the contaminated layers, and each site was then positioned on
orthophotographs at a scale of 1:40,000 and on a global position-
ing system (GPS). To assess the concentration of hydrocarbons
(C10 –C50 ), heavy metals and other contaminants involved (PCBs
and PAHs), soil samples (total of 28) were taken from the con-
taminated hydrocarbon layer. Two sampling methods were used:
the first consisted in taking soil samples (14 samples) mixed in
a receptacle to ensure the homogeneity of the sample. The sam-
ples used for the hydrocarbon-contaminated soil analysis were
refrigerated in hermetically sealed glass bottles, refrigerated at the
site and sent to a specialized laboratory where their hydrocarbon
content would be analyzed. The other samples (14 in all) were used
to analyze heavy metals, PCBs and PAHs, and were then stored in
sterile glass containers and directly refrigerated at the site. Gas
chromatography was used for the analysis of the hydrocarbon con-
centrations, with a detection limit for the C10 –C50 hydrocarbons
of 60 mg/kg of dry matter. The analysis protocol was completed
by an outside specialized laboratory (Biolab Inc.) and accredited
 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40
Fig. 1. Location on study area and spatial contamination of the riverbanks.
by the Ministère de l’Environnement du Québec (MDDEP, 2002).
For the specific sites selected for the soil and dendrochemistry
analysis, the heavy-metal (Al, As, Cd, Cu, Ni, Pb, Zn) content in the
soil samples (30 in all) was analyzed at a selective depth of the
profiles (e.g. 0–20, 20–40, 40–60, 60–80 cm) from the Richmond
site (RIC-2S and RIC-9S), the Windsor site (WIN-2S) and the Mas-
sawippi site (MAS-6S). The metal concentrations were determined
using an extraction procedure used by MDDEP (2002) and plasma
mass spectrometry (ICP-MS) was used to detect trace metal
concentrations. These analyses were done based on procedures
drawn up by the Ministère de l’Environnement (MDDEP, 2002).
Sampling of trees and dendrochemical analysis
The same three sites used for the contaminated soil profiles
were selected for the dendrochronological and dendrochemistry
analyses. These sites were also chosen for their more mature
trees and for the presence of red ash (F. pennsylvanica), a species
that is recommended for dendrochemical analysis (Bégin et al.,
1997). The sites also showed one of the highest rates of hydro-
carbon contamination along the banks of the Saint-François and
Massawippi Rivers. For each site, two tree specimens (F. penn-
sylvanica) were selected near the riverbank (less than 10 m), and
another tree (RIC-9) of the same species was selected away from
the hydrocarbon-contaminated sites (30 m of riverbank) for a com-
parison of the tree rings at the Richmond site, which has the same
environmental conditions as those found at the three sites. Sev-
eral core samples for each tree species were extracted at breast
height using a Pressler borer (5 mm in diameter). The circumfer-
ence, diameter and height of the specimen were noted, as well as
other site parameters (see Table 1). Each core sample was then
numbered, dried, sanded and polished to facilitate the counting
of growth rings under a binocular loupe (40X) and to precisely
determine the trees’ age.
For the specific dendrochemical analyses, a second group of core
samples was taken from the same seven specimens. The samples
33
were collected at chest height from all four directions (north, south,
east and west). The number of samples taken on each specimen
(5–9 cores) was based on the quantity of material obtained (mini-
mum of 5 g/tree ring). Samples were taken from ring-porous trees
(e.g. F. pennsylvanica), which are usually characterized by a low lat-
eral distribution of contaminants from one ring to another (Cutter
and Guyette, 1993), thus providing greater accuracy for the pre-
sumed year of contamination. The core samples were numbered,
dried and analyzed in the laboratory while taking care to properly
label the centre and the outside of the tree on each core sample.
The borer was rinsed with ethanol between each sample to avoid
contaminating a given sample with the previous one. Once the
dendrochronology was completed, the growth rings were removed
individually for each core using a wood blade and a binocular loupe.
The rings were grouped by year in plastic containers labelled with
the laboratory number and weighed using a high-precision elec-
tronic scale. Samples were sent to the laboratory (Trace Element
Geochemistry Laboratory CGC-Q) for dendrochemistry analysis.
The data obtained using dendrochronology allowed seven spec-
imens to be selected for dendrochemistry as soon as they were
old enough (Table 1) to provide a pre- and post-contamination
chronological series, i.e. before and after the presumed years of
contamination (around 1955 and 1963).
In the laboratory, the sequences of annual growth rings were tal-
lied manually based on the fact that the last years are known (2004
and 2005 samples). The width between the rings was measured
with a UniSlide micrometer by Velmex combined with an AcuRite
III digital counter, which allows data to be efficiently transferred to
a computer system that statistically processes the collected data.
The geochemical analyses performed on each sample pertained to
metals by ICP-MS, especially lead (Pb). This technique is generally
used to detect heavy metals in tree rings (Hagemeyer, 1995; Bégin
et al., 1997; Malawska and Wilkomirski, 2000; McLaughlin et al.,
2002; Anderson et al., 2005). Before performing the analyses, all of
the samples were placed in a solution of HNO3 and HF. The sam-
ples had to weigh at least 70–80 mg to be analyzed. The growth
34 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40

rings were analyzed separately from 1945 to 1970, which overlaps

Massawippi MASO-1/MAS-6
the presumed contamination period (between 1955 and 1963), and

Cumulic Regosol (CU.R)

additional years were analyzed for the post-contamination period.
The period from 1971 onward was analyzed two rings at a time (e.g.
273226 5022660
1971–1972, 1973–1974). Note that for the selected species, the sap-
wood/heartwood boundary corresponds to ±14 years. Moreover,

Sandy loam
3.45–6.09
0.12–1.02
49 years
certain contaminants absorbed by the tree, such as cadmium, can

35.01
spread through the other growth rings (radial translocation) that

132
5.7

16
were recently formed (e.g. 1–2 years), which could introduce a bias
in the chronology of the contamination events.
Massawippi MASO-1/MAS-1

Cumulic Regosol (CU.R) Results

273294 5022783

Concentration of hydrocarbons and heavy metals in the rivebanks

Sandy loam
3.45–6.09
0.12–1.02
64 years

The concentration of contaminants in the Saint-François and

42.02
110

Massawippi riverbanks is generally rather low, except in some

18
10

soil profiles (Saint-Laurent et al., 2008a). The C10 –C50 hydrocar-

Cumulic Regosol (CU.R)
Windsor STE-1/WIN-3

bon concentration levels in the contaminated layers range from 60

to 470 mg/kg for the selected sites. The samples taken from the
732947 5051689

Richmond (STO-10 and STO-15) and Ulverton sites (STO-14) show

the highest levels of contamination (>450 mg/kg; see Table 2). With
5.98–7.09
0.39–0.68
91 years

respect to heavy metals, 14 soil samples were analyzed, including

39.47

Loam

PCBs and PAHs. These are the same soil profiles that were used
124
21
10

for the C10 –C50 hydrocarbon analysis. The results showed very
low levels of heavy metals and polycyclic aromatic hydrocarbons
Cumulic Regosol (CU.R)
Windsor STE-1/WIN-2

(PAH), and no PCB contamination was detected. Only a few soil

samples (STO-13 and STO-15) indicate higher levels of copper and
732928 5051683

zinc in these profiles, with 120 and 130 mg/kg (Cu) and 1500 mg/kg
(Zn), respectively. Copper contamination was found in the soil sur-
5.98–7.09
0.39–0.68
74 years

face (0.5 cm) for the STO-13 profile (Saint-Nicéphore site), and at
43.30

Loam
136

a much deeper level for copper and zinc for the STO-15 profile
20
6

(Richmond site). The concentration of hydrocarbons is also high

Richmond STO-6/RIC-9a

in these samples. Some peaks (not illustrated) indicate a concen-

tration level of heavy metals found at depths of 40, 60 and 80 cm
724175 5057482

(Table 3), and two peaks with stronger concentration levels of cad-
Regosol (CU.R)

mium at depths of 100 and 180 cm in the WIN-2S soil profile, and
Sandy loam
4.71–5.38
1.10–1.44

very high concentrations of arsenic, cadmium and lead at a depth

67 years

of 220 cm in the MAS-6 profile. The soil sample (160–180 cm) of

45.84
144

profile WIN-2S containing arsenic, copper, lead, and zinc showed

31

18

concentration levels that slightly exceeded criterion A. Note that

The RIC-9 specimen is located outside of the hydrocarbon-contaminated area.
Cumulic Regosol (CU.R)
Richmond STO-6/RIC-3

this sample was taken directly from the contaminated hydrocarbon

Description of the locations, tree species and soils sampled at the study sites.

layer.
724314 5057304

Sandy loam

Dendrochemical pattern in the tree-rings

4.28–5.03
0.36–1.48
75 years

48.06
151

The dendrochemical analysis was done on the same seven

3.2

18

specimens. All the trees were old enough to cover the pre-
Cumulic Regosol (CU.R)
Richmond STO-6/RIC-2

sumed contamination event (1955 or 1963), which consists of

a hydrocarbon-contaminated layer buried in the soils of the
724376 5057125

riverbanks. Because the pollution at the different sites consists

essentially of heavy metals and petroleum products (hydrocar-
Sandy loam
4.28–5.03
0.36–1.48

bons C10 –C50 ) such as fuel or gasoline, special attention has been
68 years

43.61

given as potential markers to lead, a chemical element present in

137
16

petroleum fuels and a gasoline additive. The focus was on the lead
4

levels found in the tree’s growth rings, since lead was still used
Total organic carbon (TOC)
Age of the trees; species:
Fraxinus pennsylvanica

to manufacture petroleum products until the 1990s (CEPA, 1990).

Location site/specimens

Also, lead is in widespread use and is found in the environment. For

Distance from the

the same tree specimens, the concentration of heavy metals (e.g.

riverbank (m)
UTM (NAD-83)

Soil pH (CaCl2 )
Circumference
Diameter (cm)

Cd, Cu, Ni, Zn) was obtained by analysis. These metals are good indi-
Textural class
Height (m)

cators of industrial waste and pollution caused by human activity

Marsh.)

Soil types

and could have been present in greater or lesser quantities in the

Table 1

hydrocarbons discharged into the Saint-François and Massawippi

a

Rivers.
 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40 35

(mg/kg)

The numbers in bold indicate the level of soil contamination considering B or C criterion of MDDEP (2002). The soil with hydrocarbon (C10 –C50 ) contaminant levels ranging from 300 to 700 mg/kg falls within the criterion B;
<0.05
<0.36
<0.79
<0.16
<0.07
<0.45
<0.35
<0.36

<0.67
<0.15
<8.70

<0.06
<0.45
<0.27
PAHs
(␮g/kg)
PCBs

<10
<10
<10
<10
<10
<10
<10
<10
<16
<10
<10
<10
<10
<14
(mg/kg)
Zn

10
60
440
100
120
88
140

60
130
75
80
60
93
1500C
(mg/kg)

3.2
25.3

18.7
55
14
16
30
16
65
12
22
13
10

16
Pb
(mg/kg)

33.0
26
36
41
40
30
37
44
26
37
36
30
36
31
Ni
(mg/kg)

<0.02
0.17
0.89
0.17
0.15
0.41
0.17
0.94

0.12
0.34
<0.02

<0.06
0.15
<0.02
Hg
(mg/kg)
Cu

5
30
95
35
30

43

26
43
29
30
26
63
120B

130B
(mg/kg)

12
23
37
26
26
23
24
30
17
30
23
17
24
20
Cr
(mg/kg)

0.75
0.98
0.71
<0.03

0.21

0.59

0.19
0.60
2.90

4.90

0.50

0.30
1.3

1.0
Cd
(mg/kg)

Fig. 2. Concentration of lead in the tree specimens (a) at Richmond (RIC-2, RIC-3,
Concentration of hydrocarbons (C10 –C50 ), heavy metals, PCBs and PAHs in contaminated soil layers.

1.1

9.5
9.4

1.6

4.9

4.5
9.0
16.0

15.0
8.7
19.0

12.0

6.0
9.0

RIC-9), (b) Windsor (WIN-2, WIN-3) and Massawippi (MAS-1, MAS-6) sites.
As
Hydrocarbon

Legend for soil texture: S: sand; SL: sandy loam; L: loam; Si: silt; FSL: fine sandy loam.

Lead concentrations in the specimens

(mg/kg)

The lead concentration levels recorded in the growth rings of

<60
310
450
170
<80
<60
460
470
340
320
<80
<80
300
<60

the trees at the Richmond site show very different patterns. For
specimen RIC-2, there were four major peaks that occurred in
1948, 1951, 1954 and 1956. The year 1954 shows the highest level
1.48

1.46
0.69
0.21
0.94

0.32
0.41
0.32
0.35
0.17
0.58
0.31
0.12
TOC

of lead in the tree with a concentration of 11.38 ppm (2a). After

1966, the tree once again registered a progressive increase in lead
3.91
4.93
5.58
4.89

5.45

4.49
5.92

5.46
5.03

6.10

6.10

5.10
6.09
pH

that attained a maximum level of 2.25 ppm in 1989 and decreased

–

after 1997 to reach an average of 0.55 ppm. For specimen RIC-3,

Sand (filling material)

no significant lead increases were noted for the series, with the
exception of a very slight increase starting in 2001, correspond-
ing to an average value of 1.05 ppm from 2001 to 2005. Specimen
RIC-9 is found in the Richmond area about 30 m from the riverbank,
Texturea

outside the hydrocarbon-contaminated area. The geochemical pro-

see also Table 3 for A-B-C criteria values.
FLS

file obtained with this tree showed low concentrations in lead

SL
SL
SL
SL
SL
SL

SL
SL

SL
Si
S

(<0.4 ppm) throughout the series until 1977 (Fig. 2a). Starting in
Depth (cm)

1977, however, lead concentrations increased substantially and

levelled off at 6.29 ppm in 1987 for a rate of 0.6 ppm/year.
5–10

0.50

At the Windsor site, the lead concentration levels recorded in

5
33
60
10

28
165
32
80
10
55
13
90

the growth rings of the trees are relatively small across the series
(<0.80 ppm). For specimen WIN-2, generally stable lead concen-
MASO-1
MAS-13
STO-11
STO-12
STO-13
STO-14
STO-15
STO-10

STE-10
Profile

STO-1
STO-6

tration levels were noted from 1945 to 1957, with an average

STE-1
STE-8
STE-9

concentration of 0.07 ppm (Fig. 2b). From 1957 to 1962, lead con-
centrations increased from 0.07 to 0.61 ppm, with an average rate
Table 2

MAS
MAS
WIN

WIN
ULV

ULV
Site

of 0.37 ppm, and decreased drastically to 0.05 ppm in 1967. The

SNI

SNI
SNI
SNI
RIC
RIC

RIC

RIC

second increase in lead concentrations recorded in 1968 was equiv-

36 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40

Table 3
Heavy metal concentrations in soil profile WIN-2S at the Windsor site.

Soil profile Soil sample depth (cm) As (mg/kg) (ppm) Cd (mg/kg) (ppm) Cu (mg/kg) (ppm) Pb (mg/kg) (ppm) Zn (mg/kg) (ppm)

WIN-2S 0–20 7.20 0.39 23 18.75 85

WIN-2S 20–40 6.77 0.44 29 18.32 104
WIN-2S 40–60 6.78 0.50 34 20.31 106
WIN-2S 60–80 6.45 0.48 31 21.47 109
WIN-2S 80–100 5.89 0.57 36 26.38 119
WIN-2S 100–120 3.01 0.30 22 19.89 89
WIN-2S 120–140 4.68 0.48 28 27.96 105
WIN-2S 140–160 4.24 0.53 28 34.70 111
WIN-2S 160–180 7.16 0.81 44 50.82 144

Criterion Aa 6 1.5 40 50 110

Criterion B 30 5 100 500 500
Criterion C 50 20 500 1000 1500
a
Classification of MDDEP (2002) for heavy-metal contaminated soils. The soil classified with generic criterion A is not considered contaminated.

alent to 0.24 ppm and quickly fell back to 0.04 ppm in 1970. The
lead geochemical profile of specimen WIN-3 shows trends that
are different than those of specimen WIN-2. The levels tend to
increase throughout the series, with variations in interannual con-
centrations. An initial increase with an average rate of 0.34 ppm
was recorded in 1956 and 0.41 ppm in 1963, followed by a marked
increase in 1967 (0.61 ppm). A third major increase was recorded
between 1970 and 2000, with three peaks occurring in 1975, 1987
and 1997. During this period, metal concentrations doubled to
attain 0.72 ppm in 1987.
The lead concentration levels recorded in the growth rings of the
specimen trees (MAS-1 and MAS-6) at the Massawippi site show
dendrochemical series that differ markedly. For the MAS-1 speci-
men, some minor peaks were registered in 1943, 1951 and 1954,
and another more pronounced peak in 1949 with a lead concentra-
tion level of 1.22 ppm. However, there is a similarity between the
MAS-1 and RIC-2 curves from 1948 to 1956. For specimen MAS-
6, the series shows four moderate peaks occurring in 1967, 1973,
1989, 1995 and 2003, with a more pronounced peak in 1985. For
this year, the tree recorded the highest level of lead with a concen-
tration of 4.82 ppm. The lead level in 1985 can be compared to the
levels obtained in specimen RIC-9, which reached maximum values
in 1985 and 1987 and showed 6.17 and 6.29 ppm, respectively.
Heavy metal concentrations in the tree specimens
The dendrochemical series of the other heavy metals in the RIC-
2 and RIC-3 specimens have relatively dissimilar patterns, except
for cadmium and zinc, where levels remain relatively low through-
out the respective series. For specimen RIC-2, the concentrations
of the various heavy metals are much higher, mainly from 1948 to
1957, in particular for Al, Ni and Pb (Fig. 3a). The highest levels were
recorded in 1948, 1951, 1954 and 1956 and the geochemical curves
of aluminum, arsenic, nickel, lead and zinc are identical but with
variable concentrations. For instance, the specimen shows very
high levels for aluminum, i.e. 57220.0 ppm in 1954, whereas the
average concentration for this element is about 3169.9 ppm from
1939 to 2005, and 14780.9 ppm from 1948 to 1954 (Fig. 3b). This
period is also characterized by high levels of Ni, Zn and Pb (Fig. 2).
For specimen RIC-3, the geochemical curve differs from speci-
men RIC-2. A marked increase in Al and Ni concentrations starting
in 1979 is noted, with maximum values of up to 386.5 ppm (Al) and
11.67 ppm (Ni) in 2005 (Fig. 3c). Lastly, there was a marked decrease
in copper levels for both specimens, especially starting in 1970.
Copper levels decreased from 1002.5 to 34.8 ppm for specimen RIC-
2 and from 628.5 to 57.4 ppm for specimen RIC-3 between 1939
and 2003, respectively. With respect to specimen RIC-9, heavy-
metal concentrations are highly variable and rather low for most of
the metals (Fig. 3d). However, a significant increase in aluminum,
nickel and zinc was noted after 1975 with successive peaks in 1983,
1989, 1993 and 1997 for aluminum, in 1983, 1989, 1993, 1999, 2003
and 2005 for nickel, and in 1993 and 2005 for zinc. The significant
increase of these three elements recorded in the tree’s rings for a
given period (1975–2005) suggests a common source of pollution,
possibly associated with local or regional atmospheric pollutants.
The geochemical curves of aluminum, nickel and zinc are similar
to those of lead, which also shows a significant increase of this
element for the same period of 1975–2005 (Figs. 2 and 3), with
successive peaks in 1985, 1991 and 1995 recorded in the reference
tree (RIC-9). Lastly, with respect to copper, a progressive decrease
in this element was also noted from 1939 to 2005, from 387.77 to
42.56 ppm.
The series obtained in the growth rings of specimen WIN-2 for
the heavy metals (As, Cd, Ni and Zn) are fairly consistent with the
dendrochemical profile of lead. In fact, significant increases in alu-
minum, cadmium, nickel and zinc were noted in 1954, 1962 and
1968 (Fig. 4) similar to the series recorded for lead (Fig. 2). It is
likely that the two periods of increase in lead and heavy metals
in specimen WIN-2 (1958–1962 and 1968) correspond to two con-
tamination events associated with river spills. For specimen WIN-3,
cadmium and especially aluminum, copper, nickel and zinc con-
centrations increased substantially from 1954 to 1966, whereas
in 1967–1968, aluminum and zinc levels showed increases. The
second half of the specimen WIN-3 series shows that the alu-
minum and nickel profiles are characterized by many peaks, with
two major increases in 2001 and 2005. Copper, however, showed
a marked decline, especially after 1965.
The dendrochemical series of the heavy metals in the MAS-1
and MAS-6 specimens show similar patterns. There is a marked
and progressive decrease in copper levels for the two specimens,
especially after the 1970s. The copper concentrations that were
recorded for specimen MAS-1 decreased from 886.4 to 214.9 ppm
from 1943 to 2005 (Fig. 5a), while the concentrations for MAS-6
decreased from 973.2 to 155.2 ppm from 1958 to 2005, respec-
tively (Fig. 5b). A significant increase in nickel was also noted in the
two specimens, especially starting in 1985, along with an increase
in aluminum, especially after 1990. Concentrations of the other
heavy metals (As, Cd) remained low, with mean values of 0.44 and
0.45 ppm for arsenic, and 0.03 and 0.02 ppm for cadmium for both
specimens.
Discussion
Contamination events
Many specimen series showed continuous concentrations of
lead over time along with periodic inputs of the metal, possibly
 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40
Fig. 3. Concentration of heavy metals in the tree specimens RIC-2 (a and b), RIC-3 (c) and RIC-9 (d). The left y-axis shows the concentration of Ni and the right y-axis shows
the concentration of Al, Cu and Zn.
originating from several sources of pollution. With respect to dif-
ferent specimens, point source pollution was observed, potentially
originating from contaminated soil along the Saint-François and
Massawippi riverbanks, and probably also attributable to atmo-
spheric pollution from local or regional sources. Specimen RIC-2
shows a marked increase of lead concentrations from 1948 to 1956
(Fig. 2), with a maximum peak in 1954 (11.38 ppm). The lead pro-
file of specimen MAS-1 presents a similar curve as specimen RIC-2,
with many peaks from 1948 to 1956. For the MAS-1 specimen, the
highest concentrations of lead were recorded in 1949 (1.22 ppm).
For specimens WIN-2, WIN-3 and MAS-6, the lead concentrations
increased after this period, around 1958–1968. The peaks observed
in specimen WIN-2 from 1958 to 1962 and in 1968 suggested two
or three pollution events of some magnitude that occurred in suc-
cession. This interpretation is backed by the WIN-3 and MAS-6
specimen series where the same upward trend is noted through
many peaks from 1958 to 1968. For WIN-3 and MAS-6, a peak
was found in 1967 comparable to the peak observed in 1968 for
specimen WIN-2, though with a slight increase in lead concentra-
tions of 0.61 and 1.28 ppm, respectively. Furthermore, the reasons
for a decrease in lead concentrations recorded in specimen WIN-2
after 1970 cannot be determined, whereas specimens WIN-3 and
MAS-6 show constant absorption with many peaks, particularly in
1985–2005.
37
There is a significant increase in lead concentrations in the tree
rings of specimen RIC-9 from 1977 to 1997 (Fig. 2). This marked
increase can be attributed to atmospheric pollution. Note that spec-
imen RIC-9 is found about 30 m from the riverbank and outside
the hydrocarbon-contaminated area. If the lead profile is compared
against the geochemical profiles of the other heavy metals such as
Al and Ni (Figs. 3, 4 and 5), several similarities are in fact noted that
could indicate a common source of pollution possibly associated
with atmospheric emissions, for instance. To our knowledge, the
only major change that occurred in this area is the construction of
a new highway that began in 1973. These emissions could there-
fore come from an increase in road traffic in this area. The patterns
observed between 1977 and 1997 in the RIC-9 specimen could be
explained by a significant input in atmospheric particulates rich in
tetraethyl lead, known for being the main metal produced by road
pollution (Massadeh et al., 2004). This interpretation corresponds
to the period during which a 50-km section of highway 55 was built
from 1973 to 1980 between the municipalities of Sherbrooke and
Ulverton. The construction of the new highway inevitably led to an
increase in the use of heavy machinery during construction, which
spanned about 7 years, most likely releasing major concentrations
of heavy metals into the atmosphere, including tetraethyl lead, a
substance that was still used in gasoline at the time (CEPA, 1990).
However, specimens RIC-2 and RIC-3 did not register this lead peak
38 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40
Fig. 4. Concentration of heavy metals in the tree specimens WIN-2 (a) and WIN-3
(b). The left y-axis shows the concentration of Ni and the right y-axis shows the
concentration of Al, Cu and Zn.
(1977–1997) found in specimen RIC-9, even though the latter is
located less than 100 m from the other two specimens. However,
specimen MAS-6 also showed a marked increase in lead concentra-
tions roughly during the same period (Fig. 2). Though the precise
source of this lead contamination is still difficult to determine, it
could still be said that at least two specimens recorded a common
pollution event that may originate from a local or regional source.
For all the specimens, the analysis of the dendrochemical pro-
files reveals several contamination events along the Saint-François
and Massawippi Rivers. Metallic elements such as Al, Cu, Ni and Zn
detected in the growth rings of trees at the Richmond, Windsor and
Massawippi sites could be associated with the polluting effects of
mining and industrial activity in the area, and these pollutants may
have likely been transported by air and by the waters of the Saint-
François and Massawippi Rivers. Note that these rivers are prone to
frequent flooding and when the waters recede, the sediments are
redeposited on alluvial plains (Saint-Laurent et al., 2008a, 2010).
This may explain why the same types of contaminants are found in
the alluvial soil and in the trees in the area. Aluminum, arsenic, cop-
Fig. 5. Concentration of heavy metals in the tree specimens MAS-1 (a) and MAS-6
(b). The left y-axis shows the concentration of Ni and the right y-axis shows the
concentration of Al, Cu and Zn.
per, lead, nickel and zinc are found in different concentrations in the
alluvial soil at the Richmond, Windsor and Massawippi sites. Note
that arsenic is used to melt sulphide minerals such as copper, lead
and zinc. In fact, copper and nickel melting and refining release the
largest quantities of arsenic into the atmosphere. Therefore, these
metals may have been transported as fine airborne particles (air
emissions) or carried by the river and redeposited during succes-
sive flooding, a frequent occurrence in this area. At the Richmond
site, for instance, there was a marked increase of these metals in
the tree xylem of specimen RIC-2 from 1948 to 1954 and in 1956.
The concentrations of aluminum, cadmium and zinc also show the
same geochemical curves as those of arsenic, copper, nickel and
lead. Specimen RIC-3 has some similarities with specimen RIC-2,
particularly for Cu, Ni and Zn.
The geochemical curves of specimens WIN-2 and WIN-3 also
indicate many similarities like those of specimen RIC-2 from 1948
to 1958, with a 1- or 2-year time lag between the specimens. In
1967 and 1968, the effects of a contamination event were recorded
that was easily detectable in the trees in the Windsor (WIN-2 and
WIN-3) and Massawippi (MAS-6) sites but not recorded in the spec-
imens at the Richmond site (RIC-2, RIC-3 and RIC-9). This event
may have possibly been related to the presence of hydrocarbons
in the alluvial soil due to the combination of Ni, As and Pb, which
 D. Saint-Laurent et al. / Dendrochronologia 29 (2011) 31–40
are the main constituents of used oil and other petroleum prod-
ucts (BRGM, 2001). Note that the effects of this contamination were
recorded in 1967–1968, 4 years after the 1963 contamination event
(oil spill) which affected the Saint-François River at Sherbrooke,
according to the documents that were reviewed. This time period
may involve two processes, i.e. pedogeochemical changes and the
radial mobility of the metals in the xylem. It is also likely that
contamination events other than the 1963 event occurred along-
side the river but were not documented in the literature that was
reviewed. Other major peaks were recorded in specimens WIN-2
and WIN-3 from 1975 to 2005. The most important peaks are reg-
istered in 1974–1975, 1985–1986 and 2001–2002, in particular for
aluminum, nickel and zinc. The concentration of copper in speci-
men WIN-2 is also marked by many peaks during the last decades,
particularly in 1976, 1982, 1990 and 2004.
The appearance of heavy metals such as arsenic, copper, nickel
and zinc in the growth rings of many specimens could be asso-
ciated with industrial, agricultural or mining pollution. In fact, it
is difficult to identify the precise source or origin of the pollution
since the latter could come from different activities that are highly
diversified in the Saint-François River catchment. In addition, the
emissions of metal-bearing particles may have varied widely over
the century due to the different types of industrial activities, tech-
nological changes, and regulations on atmospheric emissions. All
of these anthropogenic changes may thus be reflected in the rings
of the trees that showed variations (Lecce and Pavlowsky, 2001;
Ciszewski and Malik, 2004). For instance, copper showed a definite
downward trend that could be attributed to a decrease in mining
in this region. However, a major increase in other contaminants
such as aluminum and nickel can be noted in most of the tree spec-
imens, especially after 1979. The progressive and constant curve
of aluminum, in particular, suggests a local or regional source of
atmospheric pollution rather than pollution originating from the
river since specimen RIC-9, which is located more than 30 m from
the rivebanks, also shows a major increase in aluminum concen-
trations. A probable source of the increase in aluminum in several
specimens may originate from the industrial activities of a alu-
minum smelter located in the Bécancour area, more than 80 km
northeast of Richmond. This industrial plant opened in 1986 and
saw a decrease in production in 2004, followed by a turnaround in
2005.
In addition to atmospheric fallout, the increase of several heavy
metals observed in the geochemical profile of the tree specimens
may also be associated with some variability in the soil pH, which
may also be linked to atmospheric fallout. Note that the soils in
this area show relatively low pH values ranging from 3.45 to 7.09
(Table 1) with mean value of 5.03. It is known that certain heavy
metals are more easily redistributed in acidic soil (Baise, 1997),
which favours a certain bioavailability of the metals found in the
soil by trees or plants (Hagemeyer, 1993; Kabata-Pendias, 2004).
It seems likely that the metal concentrations recorded in the tree
rings come from polluting atmospheric fallout that may have been
absorbed by the tree through the mineral matrix. These pollutants
were able to accumulate on the surface of the soil and penetrate the
inner layers by leaching, given that the in situ transport of contami-
nants in the mineral matrix is facilitated in acidic soil (BRGM, 2001).
This could explain why high concentrations of lead and other met-
als, including copper, nickel and zinc, are found in the subsurface
horizons.
Lastly, the analysis of the growth rings of the tree specimens
shows patterns that are irregular but that must be examined in con-
junction with the environmental conditions of these very dynamic
riverside environments (e.g. periodic flooding, redeposition of sed-
iments during flooding). In light of the results that were obtained,
the absorption patterns that were observed are relatively different
39
from one tree to another, and this variability must also be analyzed
while taking into account element mobility and availability, which
depend on several factors, including physiological responses that
can vary widely from one specimen to the next, and soil and water
characteristics, which can vary significantly over relatively short
distances. Finally, it is important to note that the Saint-François
catchment is marked by a heavy industrial past and that it is more
than likely that several contamination events occurred over the
century, especially prior to the 1970s when environmental con-
trols were virtually non-existent. It is therefore likely that several
pollution events occurred in the past but very few were recorded
in the documents that were reviewed.
Conclusion
This work shows that various contamination events were
recorded in the trees, i.e. at least two major events from 1955 to
1968, one of which may be associated with the spill of petroleum
products (hydrocabons) observed in the riverbanks (hydrocarbon-
contaminated layer). Though the trees do not always show the
same contaminant distribution pattern in the chronological series,
there is still a marked correlation between the geochemical curves
of certain specimens, including WIN-2, RIC-2, RIC-3 and MAS-1, in
particular for 1948, 1951, 1954 and 1956. This suggests that the
same contamination events were recorded by the trees. Because
of the similarity between these curves, it could be said that the
radial translocation process appears to be limited for this species.
However, other analyses will have to be done on other specimens to
confirm this hypothesis. The next stage of the study consists in con-
tinuing the work in an effort to obtain the isotopic signature of the
lead and carbon in the different hydrocarbon compounds found in
the alluvial soil samples and attempting to find new sufficiently old
tree specimens to cover the pre- and post-contamination period.
Acknowledgements
The authors would like to thank all the individuals and orga-
nizations that contributed to this study, including the Natural
Sciences and Engineering Research Council of Canada (NSERC) and
the Fond institutionnel de recherche (FIR-UQTR) for their financial
support. We would like to acknowledge the Geological Commission
of Canada (GCC-Québec) and INRS-ETE laboratory’s support for the
dendrochronology and dendrochemistry analyses, in particular Mr.
Christian Bégin, Mrs. Joëlle Marion and Mr. Stéfane Prémont. Lastly,
we would like to extend our warm thanks to Marlies Hähni, Ariane
Drouin and Marc Laurencelle for their valuable assistance during
field works.
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