Acta Oceanol. Sin., 2015, Vol. 34, No. 12, P. 147–153
DOI: 10.1007/s13131-015-0766-9
http://www.hyxb.org.cn
E-mail: [email protected]
Source identification of aluminum in surface sediments of the
Yellow Sea off the Shandong Peninsula
XU Gang1, 2, 3, 4, LIU Jian1, 2, 3, 4, PEI Shaofeng1, 2, 3, 4*, KONG Xianghuai1, 4, HU Gang1, 4, GAO Maosheng1, 4
1 Qingdao Institute of Marine Geology, Ministry of Land and Natural, Qingdao 266071, China
2 Laboratory for Marine Geology, Qingdao National Laboratory for Marine Science and Technology, Qingdao 266061,
China
3 Key Laboratory of Ministry of Land and Natural Resources for Marine Hydrocarbon Resources and Environment
Geology, Qingdao 266071, China
4 Key Laboratory of China Geological Survey Bureau for Coastal Wetland Biogeosciences, Qingdao 266071, China
Received 30 October 2014; accepted 2 March 2015
©The Chinese Society of Oceanography and Springer-Verlag Berlin Heidelberg 2015
Abstract
Surface sediment samples in the near shore area of the north Shandong Peninsula are collected for grain size and
element analyses. The results indicate that the surface sediments in the study area are primarily composed of the
silt-sized components similar to the Huanghe River. The total concentration of aluminum varies from 5.57% to
7.37% (average (6.33 ± 0.40)%), and its spatial distribution is mainly controlled by the grain size. Correlations
between the ratio of aluminum to titanium concentration and aluminum concentration, titanium concentration
and the mean grain size indicate that aluminum in the near shore surface sediments is affected majorly by the
terrigenous source, and partially by the anthropogenic source. The ratios of aluminum to titanium concentrations
are larger than the background value of loess matter at some stations due to the existence of excess aluminum
associated with human activities. Thus, the sources of aluminum should be identified firstly when aluminum is
used as an index of terrigenous matter even in the near shore area dominated by terrigenous deposits.
Key words: aluminum, source identification, surface sediments, Shandong Peninsula, Yellow Sea
Citation: Xu Gang, Liu Jian, Pei Shaofeng, Kong Xianghuai, Hu Gang, Gao Maosheng. 2015. Source identification of aluminum in surface
sediments of the Yellow Sea off the Shandong Peninsula. Acta Oceanologica Sinica, 34(12): 147–153, doi: 10.1007/s13131-015-0766-9
1 Introduction
Aluminum and titanium are the main components of continental rock, soil and weathering products, but their concentrations are very low in sea water (Taylor and McLennan, 1985).
Generally, they are extremely resistant to weathering and well
conserved in sediments (Wayne Nesbitt and Markovics, 1997;
Wei et al., 2003b), and extensively applied to estimating the contribution of terrigenous matter to marine sediments (Walsh et al.,
1988; Saito et al., 1992; Klump et al., 2000). Besides, when transportation process is considered, the ratio of titanium to aluminum concentration is helpful to trace density differences in siliciclastic matter derived from fluvial and aeolian sources (Chen et
al., 2013). Aluminum and titanium concentrations are also frequently used to normalize the other elements in order to eliminate the influence of the grain size and the source (Schropp et al.,
1990; Din, 1992). However, the excess concentration of aluminum in the calcium carbonate deposited in the equatorial Pacific
shows a positive relationship with the biogenic substances, such
as opal and carbonate, which are regularly regarded as indicators to the variation in the surface seawater productivity (Murray
et al., 1993; Murray and Leinen, 1996). The excess concentration
of aluminum and the ratio of aluminum to titanium concentration higher than the Post-Archaean average shale (PAAS) were
also found in the deep sea core sediments of the South China Sea
(Wei et al., 2003a, 2003b). However, the existence of the excess
concentration of aluminum in the near shore terrigenous deposits has been rarely reported until now. When aluminum which
contained the excess concentration of aluminum was used as an
index of terrigenous matter, it would lead to an overestimation of
the terrigenous matter if the excess concentration of aluminum
was not considered, and the aluminum will not be suitable to be
used as a reference element to eliminate the influence of the
grain size and the source as well. Therefore, it is important to
study the source of aluminum (especially, when the excess concentration of aluminum exists) in the near shore area dominated
by the terrigenous matter.
The nearshore area of the north Shandong Peninsula was
dominated by sediments from the modern Huanghe River (Liu et
al., 2002; Liu et al., 2004; Liu et al., 2007). It, therefore, was selected in this study to investigate the source of aluminum and
whether the excess concentration of aluminum existed in the surface sediment of the nearshore area dominated by the terrigenous matter.
2 Geological background
The Huanghe River substance was transported to the eastern
tip of the Shandong Peninsula by the Yellow Sea Coastal Current
(YSCC) and formed a prominent subaqueous delta dominated by
Foundation item: The National Natural Science Foundation of China under contract Nos 41406078, 41330964, 41306175 and 41206073; the
Science and Technology Development Fund Project in Shinan District of Qingdao, Shandong Province, China under contract No. 2013-14007-JY; the China Geological Survey Bureau, the Ministry of Land and Natural Resources of China under contract No. GZH201200505.
*Corresponding author, E-mail: [email protected]
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XU Gang et al. Acta Oceanol. Sin., 2015, Vol. 34, No. 12, P. 147–153
clayey silt, sandy silt and silty sand (Liu et al., 2002; Liu et al.,
2004; Liu et al., 2007). The circulation pattern of the study area is
characterized by the Yellow Sea Warm Current (YSWC) and
coastal currents in the west (Fig. 1). The YSWC, as a branch of the
Tsushima Current carrying warm and salty water, flows northwestward into the southern Yellow Sea following the Yellow Sea
Trough. In winter, when the shelf water column is nearly homogeneous, the YSWC sometimes intrudes into the northern Yellow
Sea and even into the Bohai Sea (Hu and Li, 1993). Affected by
the prevailing wind direction, coastal currents with relative low
salinity due to river influx usually flow along the coasts southward in winter and northward in summer, except the YSCC,
which flows southward persistently (Wang et al., 2001).
3 Sampling and methods
3.1 Sampling
In this study, 95 surface sediment samples were collected in
the autumn of 2004 in the Yellow Sea off the Shandong Peninsula
(Fig. 1). The surface sediment samples here conform to the top 2
Fig. 1. Schematic map of the bathymetry and regional circulation pattern in the Yellow Sea and adjacent areas during wintertime.
water depth is in meter. The square indicates the study area.
cm in the center of the box. Each sediment sample was divided
into two subsamples for the determinations of elements and
grain size analysis.
3.2 Analytical methods
3.2.1 Grain size analysis
The 95 samples were pretreated with 10% H2O2 to digest the
organic matter. The excessive H2O2 solution was removed by
heating and evaporation. After that, 0.5% of sodium hexametaphosphate was added to the samples, making the sediments disperse completely, and then the mixture was analyzed with a Mastersize-2000 laser particle size analyzer according to the same
procedure as described by Xu et al. (2014) at the Qingdao Institute of Marine Geology in China. Grain-size parameter was calculated following the method of Folk and Ward (1957).
3.2.2 Element analyses
Prior to the geochemical analysis, the samples were desalted
with distilled water and dried at a low temperature (<60°C) in a
clean oven, and then ground to 200 mesh or less in an agate mortar. The major element compositions (aluminum and titanium)
were tested by X-ray fluorescence spectrometer. To analyze the
concentrations of trace elements (barium and lead), about 100
mg of each sample was firstly digested by 1 mL 50 % HClO4 and 3
mL HF in a teflon bottle on a hotplate at about 160°C for 48 h.
After evaporation to dryness, 1 mL 55 % HClO4 was added to the
vessel, which was heated again to about 160°C until the complete
evaporation of the acid. After the sample cooled to room temperature, 1.5 mL of 50% HNO3 was added, and the sample was again
heated at 160°C for 12 h and then cooled to room temperature.
Afterwards, the solution was moved to a measuring cylinder, di-
luted with 100 mL 10% HNO3, and measured with an inductively
coupled plasma mass spectrometer (ICP-MS) (Liu et al., 2009).
To control the precision and accuracy of analyses, some samples
selected randomly were measured repeatedly and compared
with the certified reference elements, and the analytical precision for elements was generally less than 5%.
4 Results and discussion
4.1 Grain size distribution of sediments
Since aluminum is generally characterized by high affinity to
fine sediments, it tends to accumulate in the areas of low hydrodynamic energy where the fine matter is preferentially deposited.
By contrast, aluminum is diluted by coarser sediments and its
concentration becomes lower in the areas of high hydrodynamic
energy. Accordingly, grain size is a very significant factor controlling aluminum distribution in the sediment.
In our study area, the surface sediments were primarily composed of silt-sized components, with concentrations ranged from
46.7% to 72.3% (average (61.9 ± 6.6)%). The higher concentrations of these components were generally located in the near
shore area and the northwest area (Fig. 2b). The concentrations
of sand-sized components varied in a larger range from 5.7% to
43.9% (average (24.1 ± 10.1)%), and their higher concentrations
were mainly located in the eastern part (Fig. 2a). The concentrations of clay-sized components were from 6.7% to 23.8% (average
(14.1 ± 4.8)%), relatively lower than the other components in our
study area, and their higher concentrations were mainly located
in the northwest area (Fig. 2c). The mean grain size varied from
4.4Φ to 6.5Φ with an average value of (5.4 ± 0.6)Φ, which further
indicated that the surface sediments were primarily composed of
the silt-sized components (Fig. 2d). The characteristics of the
XU Gang et al. Acta Oceanol. Sin., 2015, Vol. 34, No. 12, P. 147–153
149
Fig. 2. Spatial distributions of clay-, silt-, sand-sized components and mean grain size of surface sediment in the nearshore area,
the north Shandong Peninsula.
grain size in our study area were similar to those of the Huanghe
River, since most of the sediment load of the Huanghe River is silt
and clay-sized particles derived from the Quaternary Loess Plateau as described in the previous study (Wang et al., 2015).
4.2 Chemical compositions of sediments
As shown in Table 1, the total concentrations varied from
5.57% to 7.37% (average (6.33 ± 0.40)%) for aluminum and
0.309% to 0.459% (average (0.380 ± 0.028)%) for titanium. Similarly, the total concentrations varied from 17.2 to 29.7 mg/kg
((22.6 ± 3.1) mg/kg on average) for lead and 420 to 546 mg/kg
((482 ± 26) mg/kg on average) for barium.
It is noticed that, the average concentrations of titanium and
barium in the study area are higher than those from the modern
Huanghe River Estuary, but lower than those of the upper crust.
The fact that lead concentration at some stations is higher than
that from the modern Huanghe River Estuary, loess matter and
the upper crust indicates that lead is probably influenced by human activities at some stations in our study area. The mean concentration of aluminum in our study area is significantly higher
than that in the modern Huanghe River Estuary and lower than
that in the upper crust, but close to the loess matter of the
China’s soil element background. The fact that the mean concentrations of elements in our study, especially terrigenous element
titanium, are close to the loess matter as shown in Table 1 suggests that the sediments in our study area may be sourced from
the Huanghe River, which is consistent with previous studies (Liu
et al., 2002; Liu et al., 2004; Liu et al., 2007). Although these sediments were mainly sourced from the Huanghe River, the concentrations of elements in our study area are higher than those of the
modern Huanghe River Estuary, probably owing to the fine grain
size caused by dynamic differentiation.
The spatial distribution of aluminum in the surface sediments of the north Shandong Peninsula was shown in Fig. 3. The
Table 1. Mean grain size and element concentrations of surface sediments in the study area, and comparison with those from the
other sources
Min
Max
Mean
SD
Modern Huanghe River Estuary
Loess matter
Upper crust
Mz (Ф) Al/% Ti/%
4.40
5.57 0.309
6.50
7.37 0.459
5.40
6.33 0.380
±0.60 ±0.40 ±0.028
4.90
5.28 0.335
6.27 0.380
8.10 0.420
Pb/mg·kg–1
17.2
29.7
22.6
±3.1
17.2
21.6
20.0
Ba/mg·kg–1
420
546
482
±26
413
478
550
Reference
this study
Yang and Li (1999), Yang et al. (2004)
CNEMC (1990)
Taylor and McLennan (1985)
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higher concentration of aluminum is generally located in the
nearshore area and the eastern part of the study area, and its
lower concentration is mainly located in the central part. Such
spatial distribution pattern of aluminum is consistent with that of
the mean grain size in general, suggesting that there may be correlation between the aluminum concentration and the mean
grain size. Pearson’s correlation analysis and linear regression
analysis are conducted to study the relationship between aluminum concentration and mean grain size and the result is shown in
Fig. 4. It can be seen that aluminum was positively correlated
with mean grain size (Pearson’s correlation coefficient r is 0.91,
p<0.000 1) since the concentration of aluminum increased
gradually with the increasing of the mean grain size. Accordingly,
the distribution of aluminum should be affected by the distribution of mean grain size to some extent and the high concentration of aluminum was observed in the area where fine sediment
dominated as well (as described by Fig. 2d).
Fig. 3. Spatial distribution of aluminum concentration of
surface sediment in the nearshore area, the north Shandong Peninsula.
4.3 Source identification of aluminum
4.3.1 Pearson’s correlation analysis
To identify the sources of aluminum in surface sediments,
statistical analysis with Pearson’s correlation coefficients was
conducted to get the results shown in Table 2. The enhanced
concentration of terrigenous element titanium was interpreted as
an increasing supply of fluvial siliciclastic materials or aeolian
origin in marine sediments (Arz et al., 1998; Jansen et al., 1998;
Chen et al., 2010; Chen et al., 2011). In addition, titanium was
considered to be extremely resistant to the weathering process
and a well-conserved element (Wei et al., 2003b). It is widely
known that lead is a heavy metal easy to be influenced by human
activity. Comparatively, the biogenic element of barium was easy
to be effected by biological processes, and it was usually used to
reconstruct the paleoproductivity (Schmitz, 1987; Dymond et al.,
1992).
In Table 2, a strong positive correlation was found between
lead and aluminum, indicating that aluminum had the similar
origin as lead, and thus aluminum might be influenced by human activity as well. A good positive correlation was found
between titanium and aluminum concentrations, suggesting that
aluminum was mostly from the terrigenous matter. No significant correlation is observed between biogenic element barium
and aluminum concentration, indicating that aluminum was
little influenced by biological process. In the previous study, Pattan and Shane (1999) found that aluminum concentration had a
correlation of 0.67 with titanium concentration, but no correlation with the biogenic opal, and they believed that aluminum in
the surface sediment was affected not by biological processes but
by the terrigenous and the volcanic glass in the deep Central Indian Basin. In our study area where no volcanic input existed,
matter of the surface sediment came primarily from the Huanghe
River. Therefore, the correlations between these elements concentrations probably suggest that the terrigenous and anthropogenic inputs, not the biogenic matter, made the major contributions to the aluminum accumulation in our study area.
Table 2. Pearson’s correlation coefficients for the element
concentrations in surface sediments off the north Shandong
Peninsula
Al
Ti
Pb
Ba
Al
1.000
0.675**
0.821**
–0.044
Ti
1.000
0.649**
0.161
Pb
1.000
–0.010
Ba
1.000
Notes: ** The correlation is significant at the 0.01 level (2-tailed).
Fig. 4. Correlation between mean grain size and aluminum concentration of surface sediments in the near shore
area, the north Shandong Peninsula.
4.3.2 Spatial distribution of ratio of aluminum to titanium concentrations
The ratio of aluminum to titanium concentration varied from
14.38 to 19.22 with a mean value of 16.69 in our study area. As
shown in Table 3, the mean ratio of aluminum to titanium concentration was higher than those of the modern Huanghe River
Estuary and the loess matter. In addition, the ratios of aluminum
to titanium concentrations at some stations were even higher
than the Post-Archaean average shale (PAAS). The ratios of aluminum to titanium concentrations were less than 17.00 in most
of the northwest area, and greater than 17.00 in the near shore
area (Fig. 5). The highest ratios of aluminum to titanium concentrations were distributed as circular patches in the study area,
XU Gang et al. Acta Oceanol. Sin., 2015, Vol. 34, No. 12, P. 147–153
Table 3. Comparison of ratio of aluminum to titanium
concentration in surface sediments in our study area with those
in the other matter.
Study
area
Range 14.38–19.22
Mean
16.69
Refer–
this study
ence
Modern Huanghe Loess
PAAS
River Estuary
matter
–
–
–
15.77
16.50
19
Yang et al.(2004) CNEMC
Taylor and
(1990) McLennan (1985)
Fig. 5. Spatial distribution of the ratio of aluminum to titanium concentration in surface sediments from the nearshore area of the north Shandong Peninsula.
most probably owing to some point anthropogenic pollution.
As show in Fig. 6, the ratio of aluminum to titanium concentration has no significant correlation with the mean grain size
and the total concentration of aluminum, but had noticeable
negative correlation with titanium. Since good positive correlation between titanium and aluminum concentrations has been
shown in Table 2 and titanium in the surface sediments was
mainly from the terrigenous matter, the ratio of aluminum to titanium concentration would be relative consistent to some extent if they were both terrigenous source. However, the negative
correlation between the ratio of aluminum to titanium concentration and titanium concentration in Fig. 6c indicates that the
ratio of aluminum to titanium concentration increased with the
declining of titanium concentration, probably because aluminum in the nearshore surface sediment was affected not only by
151
the terrigenous source to a large extent, but also by the anthropogenic source to a minor extent.
Shimmield et al. (1990) attributed the variation of ratio of aluminum to titanium concentration in the sediment cores from
Oman margin and the Owen Ridge in the northwest Arabian Sea
to the variation in the dust transport. However, Murray and Leinen (1996) believed that the ratio of aluminum to titanium concentration reflected the ocean productivity in the biogenic sediment dominated by calcium carbonate. Dymond et al. (1997)
suggested that the ratio of aluminum to titanium concentration
might reflect the opal rain to the seafloor as well. The study of
Pattan and Shane (1999) showed that the high ratio of aluminum
to titanium concentration was influenced by the volcanic glass.
Timothy and Calvert (1998) speculated that the high ratio of aluminum to titanium concentration was mainly resulted from authigenic clay matter.
In our study area, the sediment is sourced primarily from the
Huanghe River, and no volcanic glass input had been discovered
in history. Based on the relationship between aluminum and
lead, the correlations among ratio of aluminum to titanium concentration, aluminum concentration, titanium concentration
and mean grain size, and the spatial distribution of ratio of aluminum to titanium concentration, it is inferred that human activities might be one of the possible reasons for the higher ratios of
aluminum to titanium concentrations, since the coastal area was
densely populated and large areas of aquaculture appeared in
the nearshore area (see Fig. 5). In addition, a great amount of
waste water as a result of the rapid development of industrialization was discharged into the coastal area from surrounding areas
as well. Eutrophication was particularly serious and resulted in
the decline of water quality (Paerl, 1999, 2006). Fish farmers
spilled polymerized aluminum chloride in the culture area frequently to improve the quality of mariculture areas. Such inorganic polymer compound was capable to make organic matter
deposit quickly from seawater by a form of flocculation constituent. Anthropogenic aluminum was then deposited in the seafloor together with the flocculation constituent or transported to
the offshore area by the tide and the current, which might lead to
the higher ratios of aluminum to titanium concentrations in the
surface sediment, and the input of the excess concentration of
aluminum.
4.3.3 Spatial distribution of the excess concentration of aluminum
Traditionally, geochemists believed that aluminum in the
sediment was from the terrigenous matter. However, Murray and
Fig. 6. Correlations between the ratio of aluminum to titanium concentration and mean grain size, aluminum concentration, titanium concentration of surface sediments in the near shore area, the north Shandong Peninsula.
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Leinen (1996) found that bulk ratio of aluminum to titanium concentration of the carbonate sediments in the Equatorial Pacific
reached values up to three times over the PAAS (Taylor and
McLennan, 1985), They called it excess aluminum [ex(Al)] and
defined it as
ex (A l) = A ltot ¡ Ti sample £ (A l=Ti)PA A S ;
(1)
where ex(Al) and Altot are the excess aluminum concentration
and the total concentration of aluminum in the studied sediment, separately; and Tisample is the titanium concentration in the
sediment and (Al/Ti)PAAS is the ratio of aluminum to titanium
concentration in the Post-Archaean average shale. The source
identification of metals when compared with a global standard
was not always satisfactory because of the presence of local lithological anomalies (Zhou et al., 2014), therefore, considering the
difference in the regional background and sediment sources, the
ratio of aluminum to titanium concentration of PAAS was replaced by ratio of aluminum to titanium concentration of the
loess matter in this study. Accordingly, when the ratio of aluminum to titanium concentration in the surface sediment was higher
than the background value of loess matter, ex(Al) existed in the
nearshore area of the north Shandong Peninsula.
In the open ocean area noticeably influenced by biogenic deposits, ex(Al) mainly referred to the part of the biogenic aluminum (Murray et al., 1993; Murray and Leinen, 1996; Wei et al.,
2003a, b), comparatively, in the nearshore area dominated by terrigenous matter, it might refer to the part of the volcanic glass
(Pattan and Shane, 1999) or the anthropogenic source (especially in our study area). Although some previous studies suggested that aluminum was supplied by the terrigenous matter in the
nearshore areas (Arz et al., 1998; Jansen et al., 1998; Chen et al.,
2010; Chen et al., 2011), excess aluminum did exist in our study
area with concentrations ranging from 0% to 0.9%, and its highest
concentrations scattered generally with circular spots in our
study area (Fig. 7). In addition, its relatively higher concentrations were generally parallel to the coast with banding pattern in
the near shore area of the north Shandong Peninsula. The distribution pattern of ex(Al) was similar to the ratio of aluminum to titanium concentration, indicating that ex(Al) spatial distribution
might be controlled by the ratio of aluminum to titanium concentration associated with human activities in our study area. In
Fig. 8, ex(Al) has a very significant linear relationship with the ra-
Fig. 8. Linear regression analysis for ex(Al) and the ratio of
aluminum to titanium concentration of surface sediment
in the nearshore area, the north Shandong Peninsula.
tio of aluminum to titanium concentration (r=0.995, p<0.000 1)
based on the regression analysis, and ex(Al) increased gradually
with the raising of the ratio of aluminum to titanium concentration, suggesting that the ex(Al) of surface sediment in the study
area came mainly from the anthropogenic aluminum. Therefore,
when quantitative usage of aluminum as an index of terrigenous
materials, we should firstly ascertain whether there is ex(Al). If
ex(Al) exists, simply using total aluminum as an index of terrigenous matter would lead to overestimation of terrigenous matter.
5 Conclusions
Our study indicates that the surface sediments in the near
shore area of the north Shandong Peninsula are primarily composed of silt-sized components and their characteristics of the
grain size were similar to those of the Huanghe River. The total
concentration of aluminum varied from 5.57% to 7.37% with a
mean value of 6.33%, and the spatial distribution of aluminum
was mainly influenced by the grain size. The ratio of aluminum to
titanium concentration varied from 14.38 to 19.22 with a mean
value of 16.69, and could reach up to 19.22 at some stations
which were higher than the PAAS. The ratio of aluminum to titanium concentration was influenced not by the mean grain size
and the total concentration of aluminum, but by the anthropogenic aluminum. In addition, when the ratio of aluminum to titanium concentration was higher than the background value of
loess matter, excess concentration of aluminum associated with
human activities existed in the near shore area of the north Shandong Peninsula. In our study area, the total concentration of aluminum in the sediments might be not suitable for estimating the
components of terrigenous matter, since the existence of excess
concentration of aluminum would result in an overestimation of
terrigenous matter.
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