Anomalies of Rare Earth Elements and Heavy Metals in Modern Sediments of Small Lakes in the North of Karelia (Arctic): Geology and Technogenesis Influence

doi:10.21203/rs.3.rs-4857266/v1

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Anomalies of Rare Earth Elements and Heavy Metals in Modern Sediments of Small Lakes in the North of Karelia (Arctic): Geology and Technogenesis Influence

https://doi.org/10.21203/rs.3.rs-4857266/v1

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Lake sediments are used as indicators of the water body condition and changes that have recently occurred in it and in the it's catchment. The work examined two small lakes in Northwestern Russia (Arctic). Sediment cores were collected from the center of each lakes and separated into 1 cm layers. An ICP-mass spectrometer was used to determine the chemical composition. It was found both reservoirs have sediments containing organic matter (up to 61%). In both lakes, increased relative to the background of the region and the average content in the Earth's crust of rare earth elements, Th, V, Cr, etc. were detected. It was established that in the sediments of Lake Aprelskoe the total concentration of rare earth elements (1916 mg/kg) exceeds or is at one level with similar values for rare earth elements in lakes near cities and industrial enterprises. An analysis of the geological conditions of the study area (Karelia, Finland) showed that the source of anomalies of rare earth and other elements in the studied lakes may be bedrock containing increased concentrations of Y, Ce, La and other elements. However, an analysis of the geochemistry of the studied sediments also showed a technogenic influence on the lakes: an increase in the concentrations of Pb, Sd, Cd, Ni and Cu in the uppermost layers of sediments of lakes was established. Suspected sources of pollution are metallurgical plants in the neighboring region and the effect of long-range transport of metals due to the burning of coal around the world.

Rare Earth Elements

Heavy Metals

Geochemical Anomalies

Small Lake Sediments

Pollution

Arctic

• The REE in the sediments of a small lake is 14 times higher than the background

• Anomalies of REE in the lakes are associated with the geology of the area

• Due to long-range transport, Pb, Cd, Sb, Cu, and Ni accumulate in pristine lakes

Lake sediments can serve as indicators of various processes inside and around reservoirs. Such processes include anthropogenic influence. An increase in the content of elements as a result of anthropogenic activity, mainly as a result of the development of mining, smelting and trading activities, is recorded in lake sediments dating from the Iron Age and the time of Ancient Greece and Rome (Delile et al. 2014; Renberg et al. 1994, 2001; Carvalho and Schulte 2021; Killick and Fenn 2012; Martínez et al. 2016; McConnell et al. 2018). The peak of metal pollution was observed in European countries after World War II as a result of the reconstruction and development of cities and industry, the growth of metal production and the maximum consumption of leaded gasoline in the 1970s and 1980s (Weiss et al. 1999). For example, the effect of the use of leaded gasoline in transport operations on increased concentrations of Pb in lake sediments is known (Edgington and Robbins 1976; Escobar et al. 2013; Eisenreich et al. 1986; Norton et al. 1990; Rognerud and Fjeld E. 2001; Rognerud et al. 2013) and the influence of fuel oil thermal power plants on the appearance of technogenic anomalies V and Ni (Slukovskii 2023). At the same time, not only urban lakes or lakes near industrial enterprises can have an imprint of anthropogenic impact, but also background reservoirs that are removed from direct anthropogenic influence. This is explained by the process of long-range atmospheric transport of pollutants and their deposition at the bottom of lakes (Kusunoki and Sakata 2017). Interestingly, such a phenomenon is observed in both the Northern and Southern hemispheres of the Earth (Cooke and Abbott 2008; Shevchenko et al. 2022; Schneider et al. 2019; Vinogradova et al. 2017).

However, increased concentrations of chemical elements in lake sediments can also be influenced by natural factors, which are primarily related to the geochemical composition of rocks in the study area (Fang et al. 2023), as well as geological events such as catastrophic volcanic eruptions, such as the eruption of the Huaynaputina volcano in southern Peru in 1600, which was the strongest volcanic eruption in South America in the entire history of human settlement of the continent (Jensen 2012). Geochemical anomalies in modern sedimentary formations, which include bottom sediments of water bodies, most often occur near deposits or ore occurrences of certain elements. Previously, natural anomalies U and V associated with the manifestations of these metals in the bedrock of the studied region were noted in south Karelia (Slukovskii 2023). In general, many deposits and ore occurrences of metals, including rare earth elements (REEs), have been explored in Karelia, located on the Precambrian crystalline shield (Shchiptsov and Ivashchenko 2018).

Recently, there has been increased interest in the geochemistry of REEs in sediments and lake water, including studies of anthropogenic effects on reservoirs (Och et al. 2014; Strakhovenko et al. 2018; Wang et al. 2019; Sojka et al. 2019; Sasmas et al. 2021; Traore et al. 2023; Kreitsmann and Bau 2023; Wang et al. 2024; Gevorgyan et al. 2024). It is noted that REEs can be indicators of a negative impact on urban reservoirs, which is confirmed by paleolimnological reconstructions showing an increase in concentrations of rare earth elements in lake sediments formed during the industrial period of the development of water bodies (Slukovskii et al. 2022). In addition, REEs is an important resource for the development of a modern technological society (Goodenough et al. 2016). A successful search for deposits of rare earth metals (including geochemical anomalies in lake sediments) can lead to an economic effect, both for a single country and for the whole world.

The purpose of this work is to analyze the geochemical features of the surface sediments of two small lakes located in the northern part of the Republic of Karelia, including an assessment of the accumulation of REEs, Th, V, and heavy metals.

Description of objects and sampling

The sampling of lake sediments was carried out in 2018–2020. The сores of surface sediments from 9 lakes were collected (Fig. 1). Among the studied lakes, 4 belong to water bodies of background (pristine) territories, the others are located in the zone of influence of urban areas or industrial enterprises of the North of Russia (Murmansk, Monchegorsk, Nikel). All useful characteristics of the lakes, including main morphometric parameters and closest sources of pollution of the studied water bodies, are given in Table 1. The Garmin Echomap Plus 42cv echo sounder was used to analyze the depths of water bodies. The number of profiles for depth measurement was selected based on the size of the lakes and their shape. It is important to note that all lakes have natural glacier origin, which is typical for the North of Russia.

Lakes Aprelskoe (previously the name of the lake was used in the publication. No. 2 (Slukovskii et al. 2021)) and Permanto are small water bodies located among the northern taiga (Fig. 1). Both lakes have simple basins of slightly elongated shape. Lake Aprelskoe area is 0.03 km², the area of Lake Permanto is 0.11 km² (Slukovskii et al. 2021). The shores of the reservoirs are swampy. There is no pronounced littoral. The maximum depth of Lake Aprelskoe is 11.2 m (average 6.7 m). The maximum depth of Lake Permanto is 12.5 m (average 4.9 m). There are no cities or industrial enterprises near the reservoirs. The nearest settlement is the village of Tungozero, located a few kilometers from both lakes.

The water of both lakes belongs to the bicarbonate class and the Na group, has a very low mineralization – 11 mg/L per Lake Aprelskoe and 15 mg/l in Lake Permanto (Slukovskii et al. 2021), which is typical for reservoirs in Northwestern Russia (Kashulin et al. 2013; Filatov and Kukharev 2013). The pH value of the water is close to neutral (6.5 – in Lake Aprelskoe and 6.7 – in Lake Permanto).

The sampling of the sediments of the lakes was carried out in the summer of 2019. The sediments are represented by dark brown silts of a jelly-like consistency. The upper layers are heavily watered. Precipitation columns from the central parts of water bodies were selected using a gravity-type sampler «Limnos» (Finland). The length of the core is Lake Aprelskoe one was 42 cm, and the length of the core of Lake Permanto was 36 cm. Both cores were divided into layers of 1 cm immediately after selection. In addition, two more core from each water bodies with a length of 30 cm were selected from each lake and divided into layers of 5 cm. Then each sample was placed in a separate labeled plastic bag and then placed in a refrigerator bag for storage during transportation.

Long core with a layer-by-layer selection of 1 cm were used to analyze the total concentrations of rare elements. Granulometric analysis was performed on 5 cm samples (without destruction), and after that the samples were evaluated for the content of the main (rock-forming) elements and organic matter.

Laboratory analyzes and data processing

Granulometric analysis was performed using the LS13 320 series particle analyzer. Particles ranging in size from 0.04 microns to 2.0 mm were determined in accordance with the ISO 13320-1 standard. The analysis of the organic matter content was determined by loss on ignition (LOI), which were calculated by weight after calcination of samples at a temperature of 500°C in a muffle furnace.

To assess the chemical composition of the sediments, the samples were dried at a temperature of 100–105°C to a constant weight of the studied samples. Next, the samples were ground to a powdery state on a laboratory eraser. The oxides of the major elements (Si, Al, Fe, Na, Ca, K, Mn, Ti, P and S) were measured using the X-ray fluorescence spectrometer ARL ADVANT’X (Thermo Fisher Scientific). The content of rare and trace elements (Li, Sc, Ti, V, Cr, Mn, Co, Ni, Cu, Zn, Rb, Sr, Y, Zr, Nb, Mo, Cd, Sn, Sb, Cs, Ba, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, W, Tl, Pb, Bi, Th, U) in the samples were determined by the mass spectral method on the ХSeries-2 ICP-MS (Thermo Fisher Scientific) device. A detailed methodology for preparing samples for all these types of analysis and a description of all laboratory research methods is given in (Shelekhova et al. 2020).

In interpreting the geochemical data, the following were used: average values of elements in the upper part of the Earth's crust (Wedepohl 1995) and background levels of rare elements in lake sediments in the southern part of the Republic of Karelia (Slukovskii 2020). The MC Excel 2016 and Inkscape 0.91 programs were used to graphically represent the data.

Granulometry and major elements

Granulometric analysis of the studied lake sediments showed that the sediments of both lakes are dominated by a fraction with a particle size from 0.05 to 0.005 mm (Table 1). The median content of this fraction along the entire length of the sediments core of Lake Aprelskoe is 72.6%, and in Lake Permanto, median content of this fraction is 62.9%. Particles ranging from 0.05 to 2 mm in size in the studied sediments range from 26.6% (Lake Aprelskoe) to 36.5% (Lake Permanto). In the vertical sedimentary section, the accumulation of granulometric fractions is generally uniform. The only exception is a layer of 10–15 cm for both water bodies. In Lake Aprelskoe in this layer there was a peak in the growth of the fraction 0.005–0.05 mm and a decrease in the content of particles from 0.05 to 2 mm. In Lake Permanto, on the contrary, in this layer of the sediment core, the content of particles from 0.05 to 2 mm increases and the content of the fraction 0.005–0.05 mm decreases.

Table 1

Median contents of the main granulometric fractions and major elements in lake sediments
	Lake Aprelskoe	Lake Permanto
content of different granulometric fractions, mm
2.00-0.05	26.6	36.5
0.05 − 0.005	72.6	62.9
< 0.005	0.81	0.56
major element concentrations, %
SiO₂	35.4	41.5
Al₂O₃	4.92	1.95
Fe_total	6.75	3.47
Na₂O	0.06	0.02
CaO	0.81	0.64
K₂O	0.13	0.09
MgO	0.24	0.18
MnO	0.06	0.04
TiO₂	0.11	0.06
P₂O₅	0.64	0.23
S	0.00	0.01
LIO	50.8	51.7

The content of organic matter in the studied lakes is approximately at the same level: 50.8% (Lake Aprelskoe) and 51.7% (Lake Permanto) (Table 1). However, in Lake Aprelskoe, there is a significant variation in the values of this indicator from 25.6 to 61.1% along the core length of 30 cm. The median Si oxide content is higher in Lake Permanto sediments (41.5%) compared to sediments of Lake Aprelskoe (35.4). On the other hand, in the sediments of the Lake Aprelskoe concentration of total Fe is higher: 6.8%. A low content of Ca oxide (< 1%) was found in the sediments of both lakes. According to the classification of sediments most commonly found in the lakes of Karelia, the bottom sediments of Lake Aprelskoe refers to the organo-ferruginous type of precipitation, and the sediments of Lake Permanto have organo-silicate type (Mikhailov and Aminov 2006). Such sediments are also called sapropels. The organo-silicate type of lake sediments is the most common type of sediment in the region. Organo-glandular is less common.

Concentration of rare elements

The median concentrations of rare elements in the sediments of the studied lakes are presented in Table 2. It also shows the minimum and maximum values of each element, including a group of REEs, represented as the sum of concentrations of Sc, Y and lanthanides, from two samples. Comparison of the obtained results for rare elements with the background calculated for the southern part of the region showed enrichment of sediments of Lake Aprelskoe by Ti, V, Cr, Co, Sr, Nb, Sn, Hf, W, Tl, Th and REEs and enrichment of sediments of Lake Permanto by V, Cr, Co, Sr, Mo, Sn, Sb, W, Tl, Pb, Bi and REEs (Fig. 2). The highest concentration coefficient, calculated as the ratio of the element content in lake sediments and background (Slukovskii 2020), was obtained for REEs in Lake Aprelskoe sediments (13.7). A similar indicator for Lake Permanto is lower and is 3.8. Along with this, the concentration coefficients of V (5.5), Th (5.0), Cr (4.5) and Co (3.6) in the sediments of Lake Aprelskoe can also be considered abnormal (> 3). Also, abnormal concentrations of Tl and Co exceed 3. Previously, the authors noted increased contents of P, V, Co, Cd, Th and REEs in the sediments of Lake Aprelskoe and P, Co, Mo, Cd and REEs in the sediments of Lake Permanto relative to average content of elements in the upper part of the Earth's crust (Wedepohl 1995). In the same work, an increased concentration (2.64 mg/l) of REEs in the water of Lake Aprelskoe is noted in comparison with the background REEs content in the waters of Northwestern Russia, in particular the Murmansk region (Moiseenko et al. 2020).

Table 2

Concentrations of rare elements in sediments of the studied lakes (Me – median, Min – minimum value, Max – maximum value in the sample)
	Lake Aprelskoe			Lake Permanto
	Me	Min	Max	Me	Min	Max
Li	2.25	1.58	8.31	1.01	0.83	2.60
V	178	118	365	52	40	61
Cr	80.2	61.0	124.0	36.3	30.5	44.1
Co	21.7	6.5	120.2	28.5	9.5	44.9
Ni	8.0	5.0	32.4	7.7	6.6	16.4
Cu	17.0	4.0	56.4	23.3	19.3	28.8
Zn	90.1	30.5	157.6	73.0	56.1	115.8
Rb	4.14	3.17	25.83	3.63	2.95	9.11
Sr	43.1	35.5	99.4	38.2	34.6	49.4
Zr	29.8	21.8	110.0	8.3	6.6	13.1
Nb	1.42	1.03	3.46	0.62	0.51	1.36
Mo	1.27	0.58	3.81	4.00	2.57	8.06
Cd	0.35	0.07	1.12	0.31	0.17	0.88
Sn	0.87	0.61	3.32	0.73	0.49	2.42
Sb	0.13	0.05	1.10	0.18	0.05	1.03
Cs	0.31	0.17	0.76	0.12	0.09	0.31
Ba	248	185	539	138	116	150
REE	1051	788	1916	296	197	356
Hf	0.89	0.70	3.03	0.22	0.18	0.33
W	0.85	0.38	1.31	0.76	0.45	1.19
Tl	0.17	0.02	0.78	0.79	0.33	1.79
Pb	3.7	1.9	67.3	8.6	1.7	47.9
Bi	0.08	0.04	0.56	0.18	0.13	0.51
Th	11.1	8.6	16.4	2.2	2.0	2.6
U	1.53	1.09	2.35	0.92	0.72	1.12

REEs distribution in the sediments

Normalized diagrams of REEs distribution (lanthanides only) in the sediments of the studied lakes demonstrate similar trends in their accumulation in comparison with the upper continental crust, the Australian Postarchean shale and sediments of lakes in the south of Karelia and background lake in the North of the Murmansk region (Fig. 3). Lake Aprelskoe sediments are distinguished by a significantly higher level of accumulation of light REEs compared with other water bodies. Especially in comparison with the background level of REEs accumulation in the sediments of the south of Karelia, where organic and organosilicate sediments are predominantly found. At the same time, a similar level of accumulation of heavy REEs has been established in the sediments of Lake Aprelskoe and Lake Karkhu in the north of the Murmansk region, in which precipitation has low organic matter content, since this reservoir is located in the tundra zone (Slukovskii et al. 2022). In almost all lakes marked in Fig. 3, the REEs distribution graphs have a «negative» Eu anomaly characteristic of sedimentary formations. The sediments of Lake Permanto also have a «negative» Ce anomaly, which is also established for an unnamed lake in the north of Karelia, located several tens of kilometers from Permanto and Lake Aprelskoe (Slukovskii et al. 2021).

Analysis of the vertical distribution of rare elements in the columns of the studied lakes showed that REEs concentrations vary widely from 787 mg/kg in a layer of 24–25 cm to a maximum (1916 mg/kg) in the central part of the sedimentary section (layer 14–15 cm) (Fig. 4). In the uppermost part of the column (layers 0–10 cm), the REEs content is stable, and in the 0–1 cm layer bordering water, the REE concentration is 1002 mg/kg. A similar REEs behavior is observed in the sediment column of Lake Permanto. With variations in REE concentrations from 197 to 356 mg/kg along the entire length of the core, the maximum falls on its central part (a layer of 19–20 cm). In the upper part of the section (layers from 0 to 13 cm), there is a decrease in REE concentrations from younger layers to those formed earlier. Similarly, in the studied columns, P, V, Cr, Mn, Ba, Th, and U. Correlation analysis revealed close significant positive relationships between these elements and REEs. The highest correlation coefficients are in the REEs-V (0.96), REEs-Cr (0.96), REEs-Th (0.93) and REEs-U (0.91) pairs. Weak or insignificant correlations in the sediments of lakes Aprelskoe and Permanto are noted between REEs and elements such as Co, Ni, Cu, Rb, Cd, Sn, Sb and Pb. At the same time, these elements correlate well with each other. In particular, there is a high level of correlation in the pairs Pb-Sb (0.98), Pb-Sn (0.93), Cd-Sb (0.92), Cd-Pb (0.92), Ni-Pb (0.73) and Ni-Sb (0.72).

Comparison with polluted lakes

Studies show that elevated REE concentrations in environmental objects may indicate the influence of mining enterprises and other industries on them (Balaram 2019; Liu et al. 2019). In the Murmansk Region in northwestern Russia, a geochemical REE anomaly was noted in the sediments of Lake Bolshoy Vudjavr, which receives runoff from a local mining enterprise (Dauvalter et al. 2022). Apatite-nepheline ores, which are enriched with REEs, are mined and processed in this area to produce phosphorus fertilizers. The highest REE contents (up to 1954 mg/kg) occur in the uppermost sediment layers of Lake Bolshoy Vudjavr. In the sediments of the largest lake in the Murmansk region, Imandra, in the wastewater intake zone of this mining enterprise, a sharp increase in the amount of REEs to 959 mg/kg in a layer of 7–8 cm was recorded compared with the background value of 270 mg/kg in a core of sediments below 10 cm (Moiseenko et al. 1996, 1997; Dauvalter et al. 1999). The sediment layer with increased REE contents relative to background values in Lake Imandra is 2 times less than the sediments of Lake Bolshoy Vudjavr, which indicates a lower sedimentation rate in Lake Imandra. A similar phenomenon about the effect of phosphorus fertilizer extraction on increased REEs accumulation in sediments is described by the example of the Tagus River in Portugal (Brito et al. 2018).

Figure 5 shows that the distribution graphs of lanthanides in Lake Bolshoy Vudjavr and Lakes Aprelskoe and Permanto have similar trends, with the exception of weakly pronounced «negative» Eu and Ce anomalies in the sediments of Lake Bolshoy Vudjavr. Also, the sediments of Lake Bolshoy Vudjavr are significantly more enriched with La, Ce, Eu, Cd, Tb, Ho, Er compared with both the studied lakes and other water bodies of Russia and China experiencing anthropogenic stress. Figure 5 also shows that the total lanthanide content in the sediments of Lake Aprelskoe (969 mg/kg) is higher than in the sediments of Lake Poyang (China), which is polluted by emissions from mining and metallurgical enterprises (Wang et al. 2019), than in the sediments of Lake Aha (China), where high concentrations of REEs was influenced by coal mining (Wang et al. 2024), than in the sediments of lakes Ufimskoe and Komsomolskoe (Maslennikova et al. 2014), which are in the zone of influence of metallurgical enterprises, and then in the sediments of urban lakes of the city of Murmansk (Slukovskii et al. 2022). The median lanthanide content in Lake Permanto sediments (261 mg/kg) is also higher than in the named lakes of Russia and China, which are experiencing anthropogenic stress from various sources, including industry and transport.

Thus, the level of REE content in the sediments of lakes Aprelskoe and Permanto is close to the level of REE accumulation in the sediments of lakes in cities and industrialized regions and above the background REE level for the study region and for some background water bodies (Fig. 3). In addition, as already noted, the water of Lake Aprelskoe also has elevated relative to the background REE concentrations. All this may indicate the technogenic nature of the identified geochemical anomalies of REEs in the sediments of the studied lakes. However, Lakes Aprelskoe and Permanto are located in the background area away from any significant sources of pollution. There is also no evidence of mining of ores or other minerals in the area in the past.

Analysis of geological factors

An analysis of the geology of the study area (Fig. 6) showed that the Aprelskoe and Permanto lakes are located in the zone of distribution of the Archean tonalite-trondjemite-granodiorite (TTG) association, rocks of which are 2.8-3.0 billion years old (Shchiptsov and Ivashchenko 2018). A wider age range of these rocks is also considered: from 2.650 to 3.240 billion years (Chekulaev et al. 2021). It is known that rocks of the TTG association in the north of Karelia can be enriched with various elements, including Cr, Ni, Rb, REEs and others (Chekulaev et al. 2022). Also, several U and Au ore occurrences have been identified to the northwest of the studied lakes (indicated by numbers 1–4 on the map) (Shchiptsov and Ivashchenko 2018). To the northeast of the lake, there are outcrops of alkali-gabbro stratified intrusives with carbonatites aged from 2 to 2.07 billion years. This area is known as the Eletozersky massif or the massif Elet-Ozero (Ryabchikov and Kogarko 2015). Deposits and ore occurrences of Ce, Zr, Nb, Ta, La, Ce, Y, Zr, Hf and Be are closely related to the rocks of this massif (Shchiptsov and Ivashchenko 2018). For example, in alkaline pegmatites and metasomatites of massif Elet-Ozero, the Y content reaches 5000 mg/kg, La – 1000 mg/kg, and Ce – 3000 mg/kg (Shchiptsov and Ivashchenko 2018). The maximum values of these elements in the sediments of Lake Aprelskoe are 118.4 mg/kg (Y), 457.5 mg/kg (La) and 699.3 mg/kg (Ce).

However, it cannot be said that the entire Eletozersky massif has abnormal concentrations of REEs. Gabbroids with moderate Ti content (Ryabchikov and Kogarko 2015), normalized according to the primitive mantle (Palme, O'Neill 2014), have similar distribution trends with sediments of lakes Aprelskoe and Permanto for a number of rare elements with the exception of Th, Ce, La, Pr, Nd, Sm, Eu, Tb, Y, Tm, Yb, Lu, Rb, P and Ti (Fig. 7). The graph shows that the concentrations of REEs and Th, which also revealed geochemical anomalies in the sediments of the studied lakes, have increased values in the sediments of water bodies compared with the gabbroids of the Eletozersky massif. It is likely that the increased REE contents in this massif and in other areas of the studied territory are concentrated in acidic rocks (SiO2 > 65%). Although it is difficult to unambiguously judge from which rocks REEs and other elements correlating with them enter the water and sediments of lakes Aprelskoe and Permanto, the natural factor probably plays a key role in the appearance of the detected geochemical anomalies REEs, Th, V, Cr in the studied sediments of lakes.

About 30 REE deposits have been identified in Finland, which has a similar geology (Sarapää et al. 2013; Al-Ani et al. 2018). The highest concentrations of REEs are observed in carbonatite veins and alkaline gneiss in the central part of the country. However, almost half of Finland's REE deposits are located in the northern part of the state, including at the same latitudinal level or north of the studied lakes of Karelia. Thus, in the Sokli deposit, located in the north-east of Finland, near the border with the Murmansk region, the amount of REE in rocks reaches 18300 mg/kg (Sarapää et al. 2013). Also, increased concentrations of Th, reaching 1020 mg/kg, have been found in the rocks of this deposit.

It is also important to note that the lakes are located in front of the zone of marginal glacial formations of the Kalevala stage (Salpausselka II), represented by a wide range of diverse landforms composed of moraine, fluvioglacial sand-gravel deposits of lakes and deltas (Ekman et al. 1991). The thickness of the Quaternary deposits here reaches more than 30 meters. In the prefrontal zone in the study area, deltas are developed, with well-defined channels of thawed glacial waters, through which runoff into lakes is currently taking place. The studied small lakes, apparently of residual glacial origin, were formed after the deglaciation of the glacier in the depressions of the relief of the crystalline basement filled with well-permeable sandy sediments. It is possible that the revealed anomalies of REEs and other elements are also concentrated in the thickness of the Quaternary sediments present here.

The nature of the vertical distribution of REE concentrations in the sediment cores of lakes also speaks against the technogenic factor of REE accumulation in the sediments of Lake Aprelskoe and Permanto. Earlier, in a paper on the accumulation of REEs in modern sediments of urban lakes, it was found that under anthropogenic impact on the environment, the REE content increases from the lower layers of sediments to the upper ones (Slukovskii et al. 2022). That is, as the city grew, its industry and transport developed, there was an increase in the intake of various substances, including REEs, into the lakes of the cities of Murmansk and Monchegorsk. At the same time, no such phenomenon was observed in the background territories. In the sediments of the background lakes of northwestern Russia noted in the above-mentioned study, as well as in lakes Aprelskoe and Permanto, the REE content has peaks of elevated concentrations in both the lower and middle parts of sedimentary sections (Fig. 4). The peaks of REE concentrations in the sediment columns of the studied lakes Aprelskoe and Permanto are probably associated with granulometric the composition. In particular, a strong increase in the REE content in the middle part of the Lake Aprelskoe sediment core is explained by an increase in the proportion of siltstone and finer particles in this part of the core. It is known that REEs in sedimentary formations are well controlled by small fractions of sediments (Dubinin 2006). In the study of sediments of Lake Aha (China), increased REE concentrations were also noted in the middle part of the sediment cores, however, in this work, scientists associate this with the period of the greatest pollution of the reservoir as a result of coal mining near the lake (Wang et al. 2024).

Assessment of technogenic impact on lakes

However, the technogenic influence still affected the geochemistry of the sediments of the studied lakes. This is indicated by the distribution of some elements belonging to the group of heavy metals. For example, Fig. 8 shows an increase in concentrations of Pb, Sb and Ni in the upper layers of the sediment core of Lake Aprelskoe. The same is observed in the sediments of Lake Permanto. It was found that the maximum Pb content in the sediments of Lake Aprelskoe is 67.3 mg/kg, and in the sediments of Lake Permanto – 47.9 mg/kg. These values are 10–15 times higher than the background concentration of this metal for Karelia (4.59 mg/kg). The main source of Pb release into the environment is the use of leaded gasoline (Pacyna, Pacyna 2001). Pollution of lake sediments with this heavy metal, associated with the burning of coal in industrial enterprises, is also widespread around the world (Bindler 2000; Hosono 2016). Previously, elevated concentrations of Pb were already observed in the background territories of Northwestern Russia, including Karelia (Slukovskii et al. 2021). It has also been shown that Pb in the sediments of Karelian lakes correlates well with Sb and Cd, which also come from coal combustion as a result of long-range atmospheric transport (Krachler et al. 2005; Kuwae et al. 2013). In the Aprelskoe and Permanto lakes, these metals are similarly well correlated with each other, which indicates the influence of a technogenic factor on the appearance of geochemical anomalies Pb, Sb and Cd in the studied reservoirs. However, it is not only the burning of coal that affects the accumulation of heavy metals in the sediments of background lakes. For example, the enrichment of Ni and Cu (as well as other heavy metals, including Sb and Cd) in the upper layers of sediments of lakes Aprelskoe and Permanto is associated with the activities of metallurgical enterprises in the Murmansk region, located several hundred kilometers north of the reservoirs. It has already been demonstrated (including by the example of lakes from the Loukhsky district) that emissions from these plants can affect the chemical composition of modern sediments of lakes in Karelia (Slukovskii et al. 2021).

Lithophilic elements, including those that revealed geochemical anomalies in the sediments of lakes Aprelskoe and Permanto (REEs, Th, etc.) have a completely different distribution pattern in the studied cores of modern sediments. The lack of correlation between them and elements from the group of heavy metals (Pb, Cd, Sb, Ni) indicates different sources of their entry into the lakes. But the overall picture turns out to be a complex mixture of various factors that influenced the formation of the geochemical appearance of the sediments of the studied lakes. Previously, the authors have already noted such objects, where there is simultaneously a dominance of natural and anthropogenic factors on the chemistry of water and lake sediments. For example, in Lake Severnoe, located near the city of Murmansk, natural anomalies U and Mo were found in sediments related to the specifics of the geology of the study area (Slukovskii et al. 2020). Also, the upper layers of sediments of this water body have increased concentrations of Pb associated with emissions from motor vehicles and coal port activities, V and Ni associated with the operation of a fuel oil thermal power plant, and other heavy metals (Cd, Sb, Cu, Zn) entering the lake from anthropogenic sources.

Returning to the Aprelskoe and Permanto lakes, it is important to note that their level of heavy metal pollution is significantly lower compared to urban lakes in Northwestern Russia and lakes near industrial enterprises (Slukovskii et al. 2020). The sediments of these lakes may be of interest from the point of view of sapropel extraction, since they contain a large amount of organic matter. It is known that Karelia is rich in such a useful resource as sapropel (Mikhailov and Aminov 2006), which can be used in agriculture, medicine and other fields of human activity (Gomes et al. 2013; Blečić et al. 2014). In addition, increased REE contents may indicate a deposit or ore occurrence of these elements (or only a few elements from the REE group) in the rocks of the study area. Based on the value of REEs and the interest in their extraction (Goodenough et al. 2016; Balaram 2019), it can be recommended to continue studying this area, going beyond limnology and ecological geochemistry. However, it is still problematic to definitively establish the source of the introduction of these chemical elements into lakes. It is also recommended to pay attention to the anthropogenic impact. The work carried out can form the basis for monitoring the state of lakes in the Northwest of Russia, taking into account the vulnerability of northern and Arctic ecosystems to various environmental changes.

The sediments of lakes Aprelskoe and Permanto, located in the northern part of the Republic of Karelia, are typical sediments of small forest reservoirs in Northern Europe. The median content of organic matter in them is 51–52%. According to this indicator, the studied sediments can be attributed to sapropels, which are used in agriculture, medicine and other fields of human activity.

The uniqueness of the Aprelskoe and Permanto lakes lies in the content of rare elements in their sediments. We have established geochemical anomalies of REEs, V, Th, Cr, Co and other elements in the studied sediments. In the sediments of Lake Aprelskoe, the total REE content reaches 1916 mg/kg, which is 14 times higher than the background level for the region. The analysis showed that the median REE content in both reservoirs is at the same level or higher than REE concentrations in sediments of lakes located in cities or near anthropogenic sources. However, there are many indications of the natural origin of the identified anomalies. They are probably related to the geology of the research area. Elevated concentrations of Y, La, and Ce were previously detected in pegmatites and metasomatites of Karelia and carbonatites of the northern part of Finland.

However, anthropogenic influence has also been established in the upper layers (up to 15 cm) of sediments of lakes Aprelskoe and Permanto. We have identified increased concentrations of heavy metals (Pb, Sb, Cd, Ni, Cu), which indicates the influence of long-range atmospheric transport of pollutants. The main sources of these elements may be enterprises where coal is burned, as well as metallurgical plants. The conducted research should be continued, both from the point of view of geological interest in the search for REE sources in lake sediments, and from a conservation perspective, given that the reservoirs of the Northwest are used by people for recreational purposes.

Authors ’s contributions

ZS, VD, and TS carried out investigations, sampling, and analyses. ZS prepared the original draft of the manuscript and illustrations for it. VD, and TS had contributed to review and editing. ZS was involved in supervision and foundation.

Declarations

Conflict of interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Funding

This research is supported by the State order of Laboratory of Geoecology and Environmental Management of the Arctic of INEP KSC RAS No. FMEN-2024-0014 (study of technogenic impact on lakes), the State order of Institute of Geology KRC RAS No. FMEN-2023-0008 (study of natural impact on lakes), and also partially within the framework of the grant of Russian Science Foundation, project No. 24-17-20006 (use of data on lakes in the Murmansk region)

Author Contribution

Z.S., V.D., and T.S. carried out investigations, sampling, and analyses. Z.S. prepared the original draft of the manuscript and illustrations for it. V.D., and T.S. had contributed to review and editing. Z.S. was involved in supervision and foundation.

Acknowledgement

The authors sincerely thank the colleagues A.S. Mitsukov and M.A. Medvedev for the help with sampling, V.L. Utitsina, М.V. Ekhova, А.S. Paramonov, and S.V. Burdukh for conducting high-quality analytical studies, and M.A. Shestakov for the creation of cartographic material.

Data availability

No datasets were generated or analyzed during the current study.

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Anomalies of Rare Earth Elements and Heavy Metals in Modern Sediments of Small Lakes in the North of Karelia (Arctic): Geology and Technogenesis Influence

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Abstract

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Highlights

Introduction

Materials and methods

Description of objects and sampling

Laboratory analyzes and data processing

Results

Granulometry and major elements

Concentration of rare elements

REEs distribution in the sediments

Discussion

Comparison with polluted lakes

Analysis of geological factors

Assessment of technogenic impact on lakes

Conclusion

Declarations

Authors ’s contributions

Declarations

Funding

Author Contribution

Acknowledgement

Data availability

References

Additional Declarations

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