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Longitudinal distribution of heavy metals in fluvial sediments of the trinity River, texas.

Abstract.-A survey of fluvial sediment heavy metal concentrations (HMC) within the Trinity River was conducted to determine HMC distribution patterns and elution potential. HMC peaks associated with large population centers have been observed in Japanese rivers, most often in the downstream coastal areas where cities are concentrated. It was hypothesized that similar peaks would occur in the upper third of the Trinity River Watershed due to the influence of the Dallas/Fort Worth area. Samples were collected at 22 positions along the Trinity River during December of 2005 and analyzed for cadmium (Cd), lead (Pb), chromium (Cr), arsenic (As), mercury (Hg), nickel (Ni), zinc (Zn), and copper (Cu) content. Longitudinal HMC patterns attributable to watershed geology, hydrology, and human activity were present. The Dallas / Fort Worth mctroplex was associated with increases in HMC. Regardless of presence, all HMC in Trinity River sediments, except As, were below environmental regulatory values. Elution experiments indicated minimal leaching potential.

Trinity River sediments were surveyed from the rivers' headwaters to the Gulf coast for heavy metal concentrations (HMC) in order to determine distribution patterns and leaching potential. The position of the Dallas/Fort Worth metroplex (DFW) within the Trinity River Basin provided an opportunity to document the effect of anthropogenic sources upon background HMC distribution patterns.

As parent rock erodes, it may contain a source of heavy metal elements, which are transported downstream by surface flow and deposited within river sediments (Shimokawa et al. 1983). River sediment HMCs exhibit two general background patterns driven by watershed geology and hydrology; 1) high upstream concentrations near the source descending to lower concentrations downstream from the source or 2) a homogeneous concentration throughout the watershed. Decreasing HMC over distance can be attributed to dilution through downstream movement and sediment additions from sources lacking heavy metal content. Homogeneous HMC results from a lack of heavy metal containing parent material or a steady input throughout the watershed (i.e., homogeneous geology).

Many variables affect HMC in river sediments but human activity is a major cause (de Groot et al. 1971; Maejima & Kawasaki 2006; Wakida et al. 2008). Human effect upon HMC sediment distribution patterns is well illustrated in Japanese rivers. Peaks commonly occur near the coast where population densities are highest. Several patterns have been observed which provide a base line for quantifying human activity (Tada et al. 1984). They may be used to determine historical conditions and predict potential environmental problems (Ito & Matsumoto 2008). Mining operations, manufacturing, and urban development affect river sediment HMC (Asami et al. 1981; Giusti & Taylor 2007). Sediments from the Tama River and Tsurmi rivers in Kanagawa and Tokyo prefectures, the Shonai River in Yamagata Prefecture, and the Yahagi River in Aichi Prefecture, Japan were sampled from their headwaters to the coast and analyzed for HMC. Dilution effects were observed in the Tama River for both Ni and Cd where geological deposits in the headwaters provide heavy metal input which is then diluted through downstream transport. Japan's mountainous geography forces the majority of the population to live near the coast and, as a result, most rivers experience little HMC human influence near their source and high influence near their outflow. The Yahagi River exhibits a HMC near the outflow, a result of little or no natural heavy metal sources in the upper portions of the watersheds and a large human population near the outflow (Tada et al. 1984). As a contrast, the Tama River exhibits a dilution effect followed by a peak in the lower watershed. Peaks were observed for Ni and Cd. A flat line with a peak in the lower watershed, for NI, Cu, Zn, Cr, Pb, and Cd were seen in the Tsurumi and Shonai rivers (Tada et al. 1984). Matsumoto (2009) recently observed similar population-associated HCM peaks within Hii and Iinashi river sediments in Shimane Prefecture, Japan. Human-associated HMC peaks have also been observed in the Rhine and Ems rivers in Germany (de Groot 1971), the lower Mississippi River in the United States (Garbarino et al. 1995), the Fratta-Gorzone River in Italy (Giusti & Taylor 2007), and the Tecate River in Mexico (Wakida et al. 2009).

Several studies have documented the occurrence and levels of HMC in U.S. Gulf Coast estuary and bay sediments (Windom et al. 1989; Hanson et al. 1993; Morse et al. 1993; Sharama et al. 1999a; 1999b; Santschi et al. 2001) but none have focused on HMC distribution over a river course or watershed. This report describes longitudinal HMC distribution in Trinity River sediments from its headwaters to the coast and the influence of the DFW metroplex. Based on observations of HMC distributions in Japanese rivers, it was predicted that in the Trinity River system; 1) parent materials in the headwaters would produce both high and low HMCs, 2) HMC peaks would occur near the DFW population centers, and 3) a dilution effect would be evident above and below the urban centers. Elution experiments were conducted to determine HMC leaching potential

Materials and Methods

Study area description.-As the Trinity River flows southeasterly through Texas toward its confluence with Galveston Bay and the Gulf of Mexico, the upper-stream portion is divided into four forks: the Clear, Elm, East, and West forks. The river's length is approximately 681km from the West Fork to Galveston Bay and has a drainage area of 47,606 [km.sup.2] (USSC 1962).

The Trinity River basin geological sequence progression begins with older materials in the upper portion of the watershed and moves downstream towards newer material at the coast. The upper portion of the basin (Figure 1; Area I) is the source of eroded material that is deposited as sedimentary material as it is carried to the coast (Judy et al. 2004). Paleozoic formations of Wolfcampian, Virgilian, Missourian and Dcsmoinesian series consisting mainly of shale, sandstone, and limestone are present in the most upper portions of the basin (USSC 1962; Wermund 1996; 1999). Mesozoic groups of Trinity, Fredricsburg and L.Washita are also present (Figure 1; Area I). These parent materials provide natural sources of several heavy metals including; lead (Pb), chromium (Cr), arsenic (As), nickel (Ni), zinc (Zn), and copper (Cu). The upper middle portion (Figure 1; Area II) of the basin contains Mesozoic groups of Austin, Eagle Ford, Woodbine, Washita, Navarro and Taylor as well as Paleocene groups of Wilcox and Midway, and Eocene groups of Claiborne and Jackson (USSC 1962; Wermund 1996; 1999). These materials consist mainly of shales and limestones and contribute only small amounts of heavy metals, relative to the materials in the upper portion of the basin. The middle and lower portions of the basin (Figure 1; Area III-V) contains Oligocene formations of Catahoula, Miocene formations of Fleming and Oakvillc, Pliocene formation of Willis, and Quaternary formations of Lissie and Beaumont (USSC 1962; Wermund 1996; 1999). These formations consist of chalk, marl, unconsolidated sands, deltic sands, and muds that contribute little or no natural heavy metal elements.

[FIGURE 1 OMITTED]

Field sampling.-Twenty-two (22) sampling locations were chosen beginning in the West Fork of the Trinity River and continuing along the main segment from upstream at Jacksboro to the confluence with Galveston Bay, just south of Anahuac (Figure 1 & Table 1). Sediment sampling took place between 15 and 18 December 2005.

Sediment samples were collected within the river course and analyzed for cadmium (Cd), mercury (Hg), Pb, Cr, As, Ni, Zn, and Cu concentration. A single, representative, composite sample (-500 g dry weight) was collected from each location by combining sediments from three separate points of fluvial deposition within the reach. Samples were collected between 2 and 15 cm of the sediment-water surface interface using a 7.5 diameter by 15 cm long coring tool, homogenized by hand in a plastic bucket, placed in polyethylene sample bags, labeled, and stored on ice until delivery to Blackland Research Center in Temple, Texas. Samples were dried at 105 [degrees] C for 72 hours before being repackaged and sent to Japan for chemical analysis.

Temperature, pH, conductivity, and dissolved oxygen were measured concurrently with each sediment sampling event using a portable water probe (Model Quanta, HACH Co. Loveland, CO). Results are presented in Table 1.

Laboratory methods.--All analyses were performed by DOWA Techno-Research co., ltd., Akita Prefecture, Japan using Japanese standard methods (MEJG 2002) analogous to United States Environmental Protection Agency (EPA) methods.

Heavy metal concentration in river sediment samples was determined using batch extractions followed by spectrometry. Dried sediment samples were sieved through a 2 mm mesh screen to remove large fractions and homogenize the sample. A 3:100 sample to solution ratio was prepared by placing a 6 gram sub-sample in a disposable polyethylene centrifuge tube along with 200 mL of extractant solution. Cadmium, Pb, As, Ni, Zn and Cu were extracted using a 1 mol HC1 solution. Chromium was extracted with a 0.005 mol Na2C03 / 0.01 mol HCl solution. Samples were mixed on a linear reciprocating agitator operating at 200 cycles per minute (5 cm travel distance) for 6 hours. Following extraction, samples were centrifuged at 3000 relative gravitational fields (RGF) for 20 minutes. The supernatant was removed and filtered through a 0.45 u.m membrane filter before analytical quantification. Quantification of Cd, Pb, Ni, Zn, and Cu was done by flame atomic absorption spectrometry (EPA Method 7000B). Chromium was determined using colorimetric spectrophotometry (EPA Method 7196A), and As was quantified using hydrite generation atomic adsorption spectrometry (EPA Method 7061 A) Mercury analysis required an additional digestion. A 0.5 gram sub-sample was added to a mixture of deionized water (1 mL), concentrated nitric and perchloric acids (1:1 mixture, 2 mL), and concentrated sulfuric acid (5 mL), and heated at 200-230[degrees]C for 30 minutes. The resulting sample was analyzed using reduction vapor atomic adsorption (EPA Method 7470A).

Potential heavy metal leaching from river sediments to the water column was determined using batch water elution experiments. Nickel, Zn, and Cu were not included in the analysis. Dried sediment samples were sieved through a 2 mm mesh screen to remove large fractions and homogenize the sample. A 1:10 sample to water ratio was prepared by placing a 50 gram sub-sample in a 1 liter disposable polyethylene centrifuge tube along with 500 mL of de-ionized water. The solution was adjusted to pH 5.8-6.3 using 1M HC1 and placed on a linear reciprocating agitator operating at 200 cycles per minute (5 cm travel distance) for 6 hours. Following elution, samples were centrifuged at 3000 RGF for 20 minutes. The supernatant was removed and filtered through a 0.45 urn membrane filter before analytical quantification. Cadmium, Pb and As elution concentrations were determined by inductively coupled plasma mass spectrometry (EPA Method 200.7). Chromium was quantified using colorimetric spectrophotometry (EPA Method 7196A), and Hg was quantified with reduction vapor atomic absorption (EPA Method 7470A).

Results

As expected, HMC peaks were observed near the DFW population centers. A dilution effect was also evident above and below DFW. Lead, Cr, As, Hg, Ni, Zn and Cu concentrations generally decreased from upper portion of the watershed, increased as the Trinity River passes through the DFW metropolitan area, and then decreased again, toward the coast (Fig. 2). Cadmium showed little or no presence in Trinity River sediments (Table 1) and was above detection limit at only two points. Lead showed lower concentrations above DFW followed by a 60% increase in mean concentration (18 to 45 ppm). Immediately below the urban area, Pb concentrations decreased as sediments moved down stream and were diluted (Table 1 & Fig. 2a). Chromium concentrations were high in the upper portion of the watershed and rapidly decreased until the DFW area, where they increased again. Mean value above DFW was 28 ppm. This increased to 34 ppm within DFW. Downstream of the DFW area, mean Cr concentration decreased to 26 ppm (Table 1 & Fig. 2b). Mean As concentrations above and within DFW were the same (4 ppm), however, at the first sampling point above DFW, the value was very high (18 ppm) and the next three points were very low ([less than or equal to] 1 ppm). Concentrations below DFW showed a slight decrease with a mean of 2 ppm (Table 1 & Fig. 2c). Mercury was not detected in river sediments above DFW. Concentrations within DFW averaged 0.1 ppm. Downstream concentrations rapidly returned to below detection limits (Table 1 & Fig. 2d). Mean concentrations for Ni concentration above and within DFW were the same (12 ppm), however, above DFW, at the first sampling point, the value was very high (30 ppm) and the next four points were relatively low [less than or equal to] 7 ppm). Concentrations below DFW gradually decreased (Table 1 & Fig. 2e). Average concentrations for Zn and Cu above DFW (26 and 11 ppm, respectively) were lower than within DFW (53 and 13 ppm, respectively). Downstream dilution occurred for both metals reaching an average concentration of 29 ppm for Zn and 6 ppm for Cu. There was a large increase in Zn concentration (74 ppm) at the final sampling point (Table 1 and Figs. 2f and 2g).

All metals quantified, except As, remained bound to sediments in elution experiments. Following the 6 hour water-based elution As concentrations increased from below detection limit of <0.001 ppm and ranged from 0.001 to 0.005 ppm, well below regulatory standards.

Discussion

Naturally occurring HMC sediment sources can determined from the composition of parent material (Taylor & McLenman 1985; Condie 1993). Traversing upstream to downstream, the Trinity River exhibits HMC sediment distribution patterns which can be described as homogenous, decreasing, increasing, or both. These patterns are attributable to local geology above DFW and dilution effects below DFW. Cadmium is frequently a part of the geologic base material and can usually be detected in river sediments, but was not present in any of the samples. In Japan Cd has been documented in river sediments as results of mining operations, but recent environmental laws have reduced the problem (Asami et al. 1981; Kito et al. 1984). Relatively high values for Cr, As, Ni, and Cu were measured at the first sampling point in the Trinity River headwaters. Immediately downstream at the second sampling point, and before reaching the DFW urban area, the mean concentrations of these metals suddenly decreased by 50 to 95% (Figs. 2b, 2c, 2e & 2g). This result is explained by the presence of a reservoir directly between sampling point one and two which effectively creates a large sediment trap. Any future sampling efforts will include the reservoir in the survey.

A number of HMC peaks occur within the DFW area including; Pb, Cr, As, Hg, Ni, Zn, and Cu (Figs. 2a-g). In Japan, previous studies have made similar observations of HMC peaks associated with human population; however, they are located in the lower portion of the watershed near the coast where population centers coincide (Tada et al. 1984; Taki et al. 2001; Matsumoto 2003; Watanabe et al. 2004; Matsumoto 2005; 2009). This shift from the lower portion of the watershed, as in Japan, to the center, in Texas, is similar to results seen in Japan. These HMC peaks can be attributed to human activities such industrial or manufacturing processes.

The rise of Zn concentration near the mouth of the Trinity River may be explained by the location's close proximity to Houston, just west of its confluence with Galveston Bay. Galveston Bay itself is home to large complexes of petrochemical refining, and other industrial activity, possible sources of Zn within the system.

All but one point in this survey were below Japanese, United States Environmental Protection Agency (EPA), and Texas standards for soil HMC. The Soil Environmental Standard Values of Japan (MEGJ 2002), EPA Sediment Quality Limits (Ingersoll et al. 2000), and the Texas Risk Reduction Program - Tire 1 Sediment Protective Concentration Levels (TCEQ 2006) are shown in Table 1. One Pb measurement exceeded the EPA's sediment quality limit by 51% but it did not exceed standards set by the Japanese Government and the State of Texas. The low concentrations of these metals present no significant threat to the Trinity River ecosystem.

Elution analysis indicated that heavy metals sorbed to Trinity River sediments were not susceptible to leaching under laboratory conditions with the exception of As, which exhibited some slight desorption. At higher pH values, such as those found within the waters of the Trinity River, metals tend to remain bound to sediments (Zerbe et al. 1999). Standardized testing proeedures dietated the extracting water solution to be adjusted to pH -6.0, potentially increasing metal solubility and subsequent leaching. This was not observed, and while these results are surprising, it is beneficial, as this indicates that heavy metals should remain bound within Trinity River sediments due to the higher pH conditions (>7.5).

Conclusions

This study is the first to report HMC occurring in fluvial sediments from the Trinity River headwaters to the coast. As expected, HMC along the river course showed a variety of HMC patterns including; homogenous distributions, peaks, and peak dilutions, which were most pronounced downstream from the DFW metroplex. Dilution occurred above DFW but more rapidly than expected, and may be due to sedimentation within a reservoir between the first and subsequent sampling points. Also as expected, HMC peaks were present near the DFW metroplex and are probably due to industrial activity. All but one HMC were below environmental standards for both Texas and Japan. Elution analyses indicated that potential heavy metal leaching from Trinity River alluvial sediments is minimal.

Acknowledgments

We are greatly indebted to Shimane University and Texas AgriLife Research - Blackland Research and Extension Center - Texas A&M System for allowing us to participate in this project. We greatly appreciate Professor Takayasu, Vice President of Shimane University and Mr. Maki, Auditor of International Center for Materials Research for providing funding and support. We also thank Ms. Lisa Prcin and Dr. Rajani Srinivasan of Texas AgriLife Research / Blackland Research and Extension Center and Dr. Ikuo Takeda, Dr. Yasushi Mori and Dr. Hiroaki Somura of Shimane University for their help and support. Special thanks are extended to Mr. Jason McAlister for his assistance with site selection, sample collection, and preparation. Finally, we acknowledge the contribution of useful comments given by several anonymous reviewers and the editors.

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JW at: jwolfe@brc.tamus.edu
Table 1. Sample ID number, location description, latitude and longitude
coordinates, water quality parameters (pH, temperature, conductivity)
and concentration of cadmium (Cd), lead (Pb), chromium (Cr), arsenic
(As), mercury (Hg), nickel (Ni), zinc (Zn), and copper (Cu) from Trinity
River sediments. AH metal concentrations are reported as ppm. N/A: Not
Available.

ID Location Latitude Longitude PH Temp Cond
 description ([degrees]C) (mS/cm)

1 W Trinity 33.29 -98.08 7.60 13.0 0.208
 at Jacksboro
2 W Trinity 33.09 -97.56 7.76 16.0 0.343
 at Boyd
3 W Trinity 33.03 -97.53 7.91 15.4 0.347
 at CR 4757
4 W Trinity 32.86 -97.47 8.03 18.5 0.374
 at 10 Mi
 Bridge
5 W Trinity 32.83 -97.45 8.21 17.1 0.382
 at Lake
 Worth
6 W Trinity 32.77 -97.41 8 14 18.0 0.411
 at Hwy 183
7 W Trinity 32.76 -97.33 7.56 16.2 0.439
 at Ft Worth
8 W Trinity 32.75 -97.29 7.65 16.1 0.490
 at Ft Worth
9 W Trinity 32.79 -97.03 7.61 18.4 0.723
 at Grand
 Prairie
10 Trinity 32.77 -96.82 7.63 19.8 0.641
 at Dallas
11 Trinity 32.71 -96.74 7.56 19.0 0.590
 near Dallas
12 Trinity at 32.62 -96.62 7.53 19.5 0.059
 Belt Line
 Rd
13 Trinity near 32.43 -96.46 7.77 18.5 0.563
 Rosser
14 Trinity at 32.15 -96.10 7.63 18.5 0.556
 Trinidad
15 Trinity near 31.65 -95.79 7.80 17.1 0.820
 Oakwood
16 Trinity near 31.34 -95.66 7.98 16.7 0.786
 Crockett
17 Trinity at 30.86 -95.40 7.86 20 0 0.714
 Riverside
18 Trinity near 30.57 -94.95 8.30 19.9 0.401
 Goodrich
19 Trinity at 30.43 -94.85 8.27 19.9 0.382
 Romayor
20 Trinity at 30.06 -94.82 7.85 19.7 0.392
 Liberty
21 Trinity at 29.76 -94.69 8.14 23.1 19.00
 Anahuac
22 Trinity at 29.37 -94.78 8.01 21.2 37.70
 Galveston
 Bay

ID Location Cd Pb Cr As Hg Ni
 description (mg/Kg) (mg/Kg) (mg/Kg) (mg/Kg) (mg/Kg) (mg/Kg)

1 W Trinity <1 34 41 18 <0.05 30
 at Jacksboro
2 W Trinity <1 6 29 1 <0.05 6
 at Boyd
3 W Trinity <1 6 25 1 <0.05 7
 at CR 4757
4 W Trinity <1 30 25 1 <0.05 4
 at 10 Mi
 Bridge
5 W Trinity <1 16 19 <1 <0.05 3
 at Lake
 Worth
6 W Trinity <1 5 <10 3 <0.05 3
 at Hwy 183
7 W Trinity <1 36 35 4 <0.05 11
 at Ft Worth
8 W Trinity 2 138 46 5 0.16 13
 at Ft Worth
9 W Trinity <1 8 22 5 <0.05 14
 at Grand
 Prairie
10 Trinity <1 21 44 3 <0.05 16
 at Dallas
11 Trinity 1 61 44 4 0.20 17
 near Dallas
12 Trinity at <1 10 41 3 <0.05 15
 Belt Line
 Rd
13 Trinity near <1 23 43 5 0.07 18
 Rosser
14 Trinity at <1 12 44 2 <0.05 16
 Trinidad
15 Trinity near <1 9 43 3 <0.05 10
 Oakwood
16 Trinity near <1 <5 12 2 <0.05 3
 Crockett
17 Trinity at <1 9 39 3 <0.05 11
 Riverside
18 Trinity near <1 <5 10 <1 <0.05 <1
 Goodrich
19 Trinity at <1 <5 <10 1 <0.05 <1
 Romayor
20 Trinity at <1 <5 <10 1 <0.05 <1
 Liberty
21 Trinity at <1 8 26 2 <0.05 5
 Anahuac
22 Trinity at <1 8 <10 2 <0.05 2
 Galveston
 Bay
QSVSJ: Quality 150 150 250 150 15 N/A
Standard r
Value foSoil
of Japan (MEGJ
2002)
SQL: Sediment 3.53 91.3 90 N/A N/A 36
Quality Limits
for US soils
(Ingersoll et
al. 2000)
TPPP: Texas 1,100 500 36,000 110 34 1,400
Risk Reduction
Program-Tire
1 sediment
Protection
Concentration
Limits (TCEQ
2006)

ID Location Zn Cu
 description (mg/Kg) (mg/Kg)

1 W Trinity 51 18
 at Jacksboro
2 W Trinity 17 8
 at Boyd
3 W Trinity 21 9
 at CR 4757
4 W Trinity 26 12
 at 10 Mi
 Bridge
5 W Trinity 17 8
 at Lake
 Worth
6 W Trinity 8 4
 at Hwy 183
7 W Trinity 49 13
 at Ft Worth
8 W Trinity 86 23
 at Ft Worth
9 W Trinity 25 6
 at Grand
 Prairie
10 Trinity 61 14
 at Dallas
11 Trinity 86 20
 near Dallas
12 Trinity at 35 10
 Belt Line
 Rd
13 Trinity near 55 14
 Rosser
14 Trinity at 45 12
 Trinidad
15 Trinity near 31 6
 Oakwood
16 Trinity near 11 3
 Crockett
17 Trinity at 34 10
 Riverside
18 Trinity near 6 2
 Goodrich
19 Trinity at 4 2
 Romayor
20 Trinity at 3 2
 Liberty
21 Trinity at 19 5
 Anahuac
22 Trinity at 74 4
 Galveston
 Bay
QSVSJ: Quality N/A N/A
Standard r
Value foSoil
of Japan (MEGJ
2002)
SQL: Sediment 315 197
Quality Limits
for US soils
(Ingersoll et
al. 2000)
TPPP: Texas 76,000 21,000
Risk Reduction
Program-Tire
1 sediment
Protection
Concentration
Limits (TCEQ
2006)


Ichiro Matsumoto, June Wolfe III *, Dennis Hoffman * and Hiroaki Ishiga

Department of Geology, Shimane University Matsue, Shimane 690-8504, Japan

* Texas AgriLife Research Blackland Research and Extension Center Texas A&MSystem, Temple, Texas 76513 and Department of Geoscience, Sinmane University Matsue, Shimane 690-8504, Japan
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Author:Matsumoto, Ichiro; Wolfe, June, III; Hoffman, Dennis; Ishiga, Hiroaki
Publication:The Texas Journal of Science
Geographic Code:9JAPA
Date:Aug 1, 2010
Words:4990
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