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Groundwater Quality: Remediation and Protection (Proceedings of the Prague Conference, May 1995). IAHS Publ. no. 225,1995.

383

Environmental impact of fly ash disposal at Colorado, Illinois and Ohio test sites hydrogeological approach
JAROSLAV SOLC, H. JOHN FOSTER & RAY D. BUTLER
Energy & Environmental Research Center, PO Box 9018, Grand Forks, North Dakota 58202-9018, USA

Abstract Under the sponsorship of the US Department of Energy, the environmental impact and potential contamination from landfilled fly ash (coal conversion solid residues - CCSRs) have been studied at field sites in Ohio, Illinois, and Colorado. The progressive increase of moisture content within pilot cells over depth and time facilitated intensive chemical and mineralogical processes and generation of highly alkaline (pH of 10-12) leachate. A time-dependent decrease of Na, K, S0 4 , and CI concentration, with an attendant decline in pH and EC, corresponds to intensive leaching near the top of the ash profile and downward displacement of soluble materials toward the cell base. Potassium, chloride, pH, and EC appeared to be the most indicative parameters for tracking potential leachate transport both within the cells and below the ash/soil interface. INTRODUCTION Coal conversion solid residues (CCSRs) currently pose a serious environmental problem because of the increasingly large volumes to be disposed of and the complexity of their chemical and physical behaviour. In the past 5 years, four 2.4-m-thick test cells in three localities containing approximately 700-1000 tons each of residues were constructed. Advanced process residues from Ohio (LIMB - lime-injected multistage burner combustion process), Illinois (BFBC - bubbling fluidized-bed combustion), and Colorado (circulating FBC) were studied to assess (1) engineering behaviour, (2) chemical and mineralogical transformations of buried advanced process residues, and (3) the long-term impact of natural leaching processes on the surrounding environment. SITES CHARACTERISTICS Two cells near Lorain, Ohio, and one cell near Nucla, Colorado, were constructed in 1988-1989 followed by a cell near Canton, Illinois, in 1991. Residues were conditioned with wate r and compacted during construction. All cells were left uncovered for the first year (2 years at Illinois) to facilitate environmental interaction of disposed residues and simulate typical industrial deposition. After this initial period, cells were covered by 60 cm of compacted soil. Data on precipitation from all three localities are given in Table 1. Residues at the Ohio North cell (613 m3) and South cell (490 m3) were moisturized to 25% (North) and 35% (South) during construction, with a resultant variability in

384 Table 1 Physical parameters.


Year Precipitation (mm) 1367 830 1232 1367 830 1232 917 827 1373 214 234 233 Permeability-lab. ash soil* (cm s'1) (cm s"1) 2.5 XlO"6 1.1 XlO' 5 7.9 XlO"" 3.2 XlO' 5 1.9 XlO"6 1.5 XlO"6 5.5 XlO"6 1.5x10-" 3.9X10' 5 3.1 xlO" 5 2.3 XlO' 5 1.2x10-= 1.2 xlO' 5 2.9 XlO' 5 3.6X10' 4

Jaroslav Sole et al.

Ash-Guelph permeameter (cm s'1) 1.4x10" 1.0x10" l.lxlO4 8.0x10-" 8.5x10'" 3.1x10-" 1.1 xlO- 3 3.9x10-" 1.5x10-" 7.9x10'" 8.4x10-"

Moisture ash soil

ash**

(%) (%)
30 60 73 89 33 42 52 84 41 50 79 18 20 24 26 9 10 12 11 9 7 14 10 17 27 21 13 16 11 10

( % )
60 51 73 46 40 60

Volumetric Compressive moisture***: strength (MPa) ( % ) 67 59 57 62 65 62 47 63 75 23 24 26 4.9 3.9 5.2 2.4 7.7 6.2 5.6 2.1 2.3 1.1 0.4 3.2 3.4 3.0 3.7

1989 1990 1991 1992 1989 1990 1991 1992 1991 1992 1993 1989 1990 1991 1992

2.1 XlO' 6

2.1 xlO' 6

1.7 XlO'

2.8 XlO"8

* Average values from 1989-1992 (1991-1993) Illinois. ** Lab averages to depth of 1.8 m. *** Volumetric moisture - measurements from neutron access tubes to depth of 1.8 m at Ohio, and 2.4 m at Illinois and Colorado.

compaction and moisture build-up. Relatively high precipitation, the porous nature of the residues, and low permeability of surrounding soils (Table 1) facilitated early saturation and intensive leaching processes within the cells. The pilot cell at Illinois, containing 384 m3 of BFBC residues moisturized to 26%, was emplaced in a reclaimed part of a surface mine. In spite of precipitation similar to that in Ohio, it took about a year to achieve saturation sufficient to allow for pore-water sampling. Semiarid conditions at the Colorado site (Table 1) prevented sufficient saturation for pore-water sample recovery. Residues (612 m3) were conditioned on the average to 22%. MONITORING Each cell was instrumented with as many as 20 pressure vacuum soil lysimeters, four neutron access tubes, and runoff collectors. Nests of upgradient and downgradient monitoring wells were installed at Ohio (eight wells) and Illinois (nine wells). The sampling schedules and measurements were conducted on a quarterly basis during the first year, followed by annual sampling of fly ash and soil cores and measurements of volumetric moisture content (neutron probe) and field-saturated hydraulic conductivity (Guelph permeameter). Water samples from monitoring wells and lysimeters were collected on a quarterly basis. ASTM (American Society for Testing and Materials) standard leaching tests, X-ray fluorescence bulk analyses (XRF), X-ray diffraction mineralogical analyses (XRD), and some key engineering tests (moisture, permeability, unconfined compressive strength, etc.) were performed on selected ash and soil cores. This intensive data collection effort is based on a common-sense model, which tracks changes in mineralogy and chemistry of waters percolating through the cells in

Environmental

impact of fly ash disposal at Colorado, Illinois and Ohio test sites

385

Surface Water OHSW -E 1LSW -t ash - ASTM 9 1NC7-6 IS 9 1SC3-6 IISE 92IL1-6 9 1NC5-17 IE 9 1SC3-17-jp 92IL1-12- Lysimeters 9 1NCLY-2 90SCLY- I I 93ILLY- 5-E 92NCLY-24 92SCLY-25-t 93ILLY- 14 900HMW-3900HMW-8 92ILMW-2 92ILMW-50

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Na H K D Ca H Mg S04 Q HC03/Balance H CI Fig. 1 Typical chemistry of water at Ohio and Illinois test sites.

time and assesses the quality and extent of the resulting impact of highly alkaline leachates on the environment. Figures 1 and 2 show the typical chemistry of the waters in Ohio and Illinois selected to represent mean values, illustrating the movement and evolution of water from the surface of cells downward to lysimeters and finally to monitoring wells.
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386

Jaroslav Sole et al.

RESULTS Ash composition and mineralogy Coal used at the Ohio Edgewater power plant (LIMB) at the time of cell construction had an ash content of slightly over 10% and a sulphur content of about 2.5% (Weinberg & Petrini, 1993). The bulk composition of ash averaged about 40 % CaO, 23% Si0 2 , 13% S0 3 , and 9% of both Al 2 0 3 andFe 2 0 3 . The Illinois Midwest Grain power plant (BFBC) coal had 3.1% sulphur and about 10 % ash, with resulting residues containing about 50 % CaO, 20% Si0 2 , 12% S0 3 , and about 6% Al and Fe oxides. The Colorado Ute plant burned low-sulphur (0.75%) coal containing 16.5% ash. Residues consisted of 15% CaO, 47% Si0 2 , 23% A1203, 7% S0 3 , and 3% Fe 2 0 3 . There were no significanttimeor depth-related trends observed, except at the ash/soil interface, and slight changes in amounts of certain oxides results from variations in coal quality and combustion conditions. Unlike the "conservative" nature of bulk chemical composition, cementitious and hydration reactions resulted in significant new crystalline phases detected by XRD and scanning electron microscopy (SEM) techniques (Butler el al., 1993). Depending on available moisture, anhydrite in the initial ash may be transformed to gypsum within a short time. As shown in Fig. 3, new phases, such as ettringite (25-30%) and thaumasite (0-30 %), which crystallize under high-sulphate conditions (Crammond, 1985), dominate the mineralogy of the Ohio residues. Gypsum shows a slightly negative trend (from 7% to 1.5%) over time. Illinois residues contain approximately an equal share of gypsum and ettringite (26%), with a substantially higher content of portlandite (12-18%) than Ohio residues. Insufficient moisture in Colorado resulted in an excess of unreacted lime (30-40%) and a relatively high proportion of residual anhydrite (3%) with respect to gypsum (3-5%).

1989 1990 199 1 1992 1989 1990 199 1 1992 Fig. 3 Ohio mineralogical trends (XRD average values).

Physical parameters Physical parameters measured in the laboratory and in the field (Table 1) greatly influence the potential for, and intensity of, leachate generation. Laboratory permeabilities and field Guelph permeameter values differ by approximately one to two orders of magnitude and, in general, indicate a higher permeability in compacted

Environmental impact of fly ash disposal at Colorado, Illinois and Ohio test sites

387

residues than surrounding soils. This is attributed to formation of microfractures as a consequence of mineralization, dissolution and precipitation reactions, and freeze-thaw processes. Progressive increases in moisture content with depth and time, with maximum values near the ash/soil interface, indicated moisture build-up toward the bottom of cells at Ohio and Illinois. Dynamic physical processes, accompanied by intensive leaching, result in a general decrease of compressive strength of bulk ash with time (Table 1). Leachate quality characteristics and trends Although initially low permeabilities slowed the downward migration of strongly alkaline pore waters (pH 10-12, EC 4-8 mS), saturation increased over time, and samples were collected in the vacuum pressure lysimeters. A time-dependent decrease of Na, K, S0 4 , and CI concentration (Figs 4 and 5), with an attendant decline in pH and EC in the upper part of the cell, contrasts with increasing concentrations in samples from the lower part of the cell and below the ash/soil interface. The concentrations of these ions were highly variable, depending on lysimeter environment and depth. However, obvious trends in the chemistry of samples from each lysimeter have been observed. Potassium, chloride, pH, and EC appeared to be the most indicative of leachate transport at the Ohio site, both within the cells and under the ash/soil interface (Figs 5 and 6). Increased potassium concentrations and increased pH and EC in ASTM soil leachate analyses have been observed approximately 40-60 cm below the bottom of cells, which might support an estimation of the rate of vertical contaminant transport. While sulphate and sodium showed trends similar to those of potassium and chloride, calcium concentration remained more stable both in depth and time. The Ohio and Illinois monitoring nests, consisting of vertically staggered wells, are located about 10 m upgradient and downgradient from the cells. Groundwater levels at

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388
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Jaroslav Sole et al.

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meq/L Fil ;. 5 Ohio - North cell - ASTM leachate chemistry trends, 1990 to 1992.

the Ohio site are about 2-3 m below the bottom of the cells and have fluctuated about 1-1.6 m during monitoring since 1989. Na, Ca, Mg, S0 4 , and CI ions dominate groundwater chemistry. The presence of chloride indicates possible contamination of downgradient wells. However, only the shallowest well (OHMW-6,5 m) shows a steady increase in chloride concentration. To date, similar trends have not been shown by other ions, pH, or EC. Groundwater levels in monitoring wells in Illinois are about 0.5-2 m below the bottom of the cell and have fluctuated about 1.6 m within the observed period (1991-1993). Na, Ca, Mg and S0 4 have been very stable over time, both in upgradient and downgradient wells. As in Ohio, only the shallowest well (ILMW-3, 5.3 m) experienced a slight increase in chloride concentration. However, with regard to the

Environmental impact of fly ash disposal at Colorado, Illinois and Ohio test sites

389

Fig. 6 Ohio - North cell - ASTM leachate pH trends with depth and time.

natural variations of CI anion concentrations in this reclaimed mine, any conclusion on contribution from the ash cell is tentative at this time. CONCLUSIONS Pilot-scale field experiments, supported by intensive monitoring and analyses, indicate that even "dry deposition" of coal combustion residues can have a significant potential to contaminate soils and water. With time, increasing moisture content within the landfill from precipitation and infiltration allowed for the generation of a highly alkaline leachate (pH of 10-12), which migrated from the landfill cells to surrounding soils. Na, K, S0 4 , and CI ions, together with pH and EC, were useful indicator parameters for monitoring leachate behaviour and migration. The rate of transport and chemistry of leachate depend upon interrelated mineralogical, physical, and chemical conditions, particularly on the initial quality of the combustion residues, climatic conditions, methods of deposit and containment, ash and soil permeabilities, and site geology and hydrogeology. Acknowledgements This project was sponsored by the US Department of Energy Morgantown Energy Technology Center with overall project management by Radian Corporation. Technical assistance inXRD mineralogy by G. J. McCarthy, NorthDakota State University, is gratefully acknowledged. REFERENCES
Crammond, N.J. (1985) Thaumasite in failed cement mortars and renders from exposed brickwork. Cement and Concrete Res. 15, 1039-1050. Butler, R.D., Brekke, D.W., Foster, H.J., Sole, J. & McCarthy, G.J. (1993) Mineral transformation in buried FBC ash and effects on long-term physical and chemical behaviour. In: Proc. of the 17th Low Rank Fuels Symp. (St. Louis, USA). Weinberg, A. & Petrini, R.H. (1993) Advanced coal technology waste disposal. Ohio LIMB site assessment report. Radian Corporation, Austin, Texas.

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