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IVastc Management & Research (1988) 6, 227-238

HEAVY METAL LEACHABILITY FROM SOLID WASTE


INCINERATOR ASHES

S. E. Sa~vell, T. R. Bridle and T. W. Constable*

(Receit'ed October 1987)

The leachability of heavy metals in municipal solid waste (MSW) incinerator residues
was evaluated using equilibrium leach tests and the sequential chemical extraction
procedure. Incinerator bottom ash, boiler and economizer fly ashes were sampled
from a full-scale two-stage combustion facility without pollution-control devices. Fly
ashes were also collected from a pilot-plant scale, lime-based flue-gas scrubber
system, connected to a mass burning incinerator facility. Generally, bottom ashes
contained low to moderate concentrations of cadmium, copper, lead and zinc which
are relatively insoluble under normal landfill leaching conditions. Fly ashes contained
relatively moderate concentrations of cadmium and copper and much higher con-
centrations of lead and zinc which are readily available for leaching under normal
landfill conditions. Metal leachability appears to be dependent upon metal
speciation, the pH of the leaching medium and ash particle size.

Key Words--I.eachability, heavy metals, MSW incinerator ash, speciation, lime


scrubbing, lead, cadmium, copper, zinc.

!. Introduction

The recent increase in the utilization of incineration technology in the management of


municipal solid waste (MSW) and the implementation of more efficient air-pollution
control technologies has resulted in increased quantities of ash being collected at energy-
from-waste (EFW) filcilities. MSW ashes are currently being iandfilled in a simihtr
manner as benign industrial ashes; however, concern has been expresscd by some
government agencies and environmental groups over such disposal practices for these
residues.
Although numerous studies have been conducted on the fate of heavy metals in
ashes from coal-fired generating stations ( G o l o m b 1978; Phtmg et aL 1979; Constable
& Ross 1986; Constable & C6t6 1986; Constable & Sawell 1986) and from incinerated
sewage sludge residues (Dewling et al. 1980; Campbell et aL 1982; Bridle et al. 1987),
the literature on leachability studies conducted on MSW ashes is very limited. Hence
the environmental ramifications of hmdfilling EFW ashes are largely unknown.
To assess the suitability of MSW incinerator ashes for iandfilling and to assist in the
development of solid waste management criteria for their ultimate disposal, a series of
studies was initiated in 1984 at the Wastewater Technology Centre (WTC), under
Environment Canada's National Incinerator Testing and Evaluation Program
(NITEP). This paper describes the results of two leachability studies conducted on
residues generatcd at two Canadian EFW facilities, which differcd both in operational
design and pollution control tcchnology.

* Environment Canada, Environmental Protection, Wastewater Technology Centre, Burlington, Ontario,


Canada.
228 S.E. Sawell et al.

E
8

-7.
0

.,.d

u~

0
e,
0
..d

~u
Heatg" metal leachability 229

2. Incinerator design

2. I Prhwe Ethrard Isla~td energy from waste facility


The first incinerator tested under N I T E P was the Prince Edward Island Energy From
Waste facility (PEI-EFW) located in Parkdale, P.E.I. Testing occurred during the fall
of 1984. The facility is classified as a two-stage combustion design consisting of three
Consumat CS.1600 incinerators with a total capacity of 100 tonnes of garbage per day.
A common exhaust manifold leads to a waste heat recovery boiler, followed by an
economizer. The gases are then discharged to the stack via an exhaust fan. A process
schematic of the facility is given in Fig. 1.

2.2. Flakt air polh/tion control pilot phmt


Phase II of N I T E P was conducted during the fall of 1985 and involved testing at the
Quebec Urban Community (QUC) MSW incinerator facility. This incinerator is clas-
sified as a mass burn design capable of handling 227 tonnes of garbage per day in each
of its four parallel units. A schematic of the facility is given in Fig. 2. An air pollution
control (APC) system pilot plant was built by F L A K T Canada adjacent to the Q U C
facility, where it took a slipstream of the incinerator gases from the electrostatic
precipitator inlet. The pilot plant was configured to operate as two different types of
air-pollution control systems, a wet-dry system and a dry system. Both systems utilized
a lime-based scrubbing process followed by a fabric filter dust collector. A schematic of
the pilot plant is shown in Fig. 3. In the dry system, flue gases from the incinerator
entered a wet~lry scrubber where the gases were cooled with a water spray. The gases
then passed into a dry scrubber vessel where dry hydrated lime was injected into the
gas stream with compressed air. The flue gases, with the entrained dry lime products,
then passed through a fabric filter dust collector as the final stage of pollutant removal.

FLUE GASES
I
STAGE ELECTROSTATIC
PREC~ITATOR

STACK
WATER WALL SECTION

AUXILIARY FUEL

CRANE OPERATOR BOOTH - - ND~JCED DRAFT FAN

VERT!CAL TUBE
BOILER SECTKM
VIBRATING FEEDER
HOPPER

/
1[ REFRACTO Y FU N CE

REFUSE STORAGE PIT

ASH G4JENCH TANK AND


DRAG CHA=N

Fig. 2. Quebec incinerator schematic cross-section.


230 S. b~: Sawell ct al.

OUTLET(STACK)......_~ .

2K.L~qAy

INLFT
SAMPUNG ~"

AT~
FILTER

LOCATION

Fig. 3. Processschematicsof Flakt's two pilot plant air-pollutioncontrol systemsat Quebec.

In the wet-dry system, flue gases were contacted with a lime slurry spray in a wet--dry
scrubber vessel for chemical conditioning and cooling. The gases then passed through
the fabric filter unit, bypassing the dry scrubber vessel.

3. Sample collection
Twelve performance tests (PTs) were conducted at the PEI-EFW facility, representing
four sets of operating conditions run in triplicate (Table I). Samples of ash (bottom,
boiler and economizer) were collected from one of the test runs under each set of operating
conditions. Thirteen performance tests were conducted at the FLAKT pilot plant under
six different sets of operating conditions (Table 2). Ashes from the wet-dry scrubber
vessel, the dry scrubber vessel and the fabric filter unit were collected from one of the
test runs under each set of operating conditions. In runs PT7 to PTI0, no dry scrubber
ash was collected because the dry scrubber vessel was bypassed during the wet--dry
system testing.
Detailed information on the operational design and the operating conditions of both
facilities, are given in the NITEP Summary Reports (Environment Canada, 1985, 1986).

4. Experimental and analytical procedures


Ash samples from both facilities were analyzed for their total heavy metal concen-
trations using standard analytical techniques. Prior to digestion with aqua-regia and
hydrofluoric acid, the ashes were dried and then ground to pass through a No. 100
(150 itm) mesh sieve. The metal concentrations in the ash samples and leachate were
measured using inductively coupled argon plasma (ICAP), flame atomic absorption
(AA) or AA with graphite furfiace.

4.1. P E I - E F I V ashes
PEI-EFW ashes were subjected to the WTU Multiple Batch Leaching Procedure
(MBLP) (Constable & C6t6, 1986). The test involved exposing the samples to three
ltea O' metal leachabili O' 231

TABLE 1
PEI-EFW incinerator operating conditions

Settings
Operating Primary temp. Secondary temp. Feed cycle Performance
mode (~ (~ (rain) test no.

Normal operation 695 1000 8.7 3


Low feed rate 690 1000 12 5
High temperature 700 1135 8.7 9
Low temperature 675 900 8.7 12

TABLE 2
Flakt pilot plant operating conditions

Temperature before fabric filter (~

Performance
Operating mode Target Actual* test no.

Dry system 200 209 6


140 141 2
125 125 4
!I0 113 12

Wet~lry system 140 140 8

( + Recycle) 140 141 10

* Thermocouple data from pilot plant control system.

different types of leaching media (distilled water, an acidic solution and a synthetic
municipal landfill ieachate) at a liquid-to-solid ratio of 20: I. The solids and leaching
media were then rotated at 2-3 rpm for a period of 18 h. After a short settling period,
the supernatant was decanted and filtered through a 0.45 ltm membrane filter. Each
leachate was measured for pH, conductivity, and total dissolved solids (TDS) before
being preserved with concentrated nitric acid to a pH of 2 and analyzed for heavy
metals. Results from the M B L P are given in terms of fraction extracted, which is defined
as the ratio of the mass of a metal in a leachate to the mass of that metal in the ash
sample, expressed as a percentage.

4.2. Flakt pilot plant


The fly ashes collected from the Flakt pilot plant were subjected to a limited MBLP.
Only a distilled water batch leach was used. T h e s e ashes were also subjected to a
sequential chemical extraction (SCE) procedure which determines the speciation and
total concentration of the heavy metals under consideration (Fraser & Lum 1983). The
procedure involved a step-wise separation of the total mass of a metal in an ash sample
into five fractions. Fraction A (the ion exchangeable fraction) was determined by ext-
racting the ash with a ! M solution of LiCI/CsCI. The residue from Fraction A was then
extracted with an acetic acid solution buffered with sodium acetate to determine Frac-
tion B (the surface oxide or carbonate bound metal ions). Ill Fraction C, the iron and
232 S.E. Sawell et al.

50000
ECONOMIZER ASH
~,uz,-,,,,~ BOILER ASH
r,,.,'/,,-J BOTrOM ASH
E 40000
Q.
rl

z 30000
0
I.-
<
r
}-" 20000
z
I.d
Z
0 10000
0

.......... [7771 !

Cd Cu Pb Zn
HEAVY METALS
Fig. 4. Average heavy metal concentrations in ashes from the P E I - E F W facility.

manganese bound metal ions were extracted from the remaining residue using 0.4 r,t
hydroxylamine hydrochloride in 25% (v/v) acetic acid. In Fraction D, the organically.
bound metal ions and sulphides were leached from the residue remaining from Fraction
C by extraction with 0.02 M nitric acid and 30% hydrogen perixode. Finally, Fraction E
was extracted from the remaining residue of Fraction D, using a total digestion with
a~lua-regia/hydrofluoric acid and hydrogen perixode, giving the residual metal ions.

5. Results.and discussion

5.1. P E I - E F W facility
5. I.I Metal concentrations ht ashes
The average concentrations of cadmium, copper, lead and zinc in the MSW ashes from
the PEI-EFW facility are shown in Fig. 4. Typically, the bottom ashes contained low to
moderate concentrations of cadmium, copper, lead and zinc, ranging from 30 ppm for
cadmium to 5900 ppm for zinc. Higher concentrations of copper were found in the
bottom ashes (average of 1500 ppm) than in the fly ashes (average of 555 ppm). In
contrast, the boiler and economizer fly ashes contained very high heavy metal con-
centrations, especially lead and zinc (up to 3.6% for Pb and 5.4% for Zn).

5.1.2. Leachabilio'
The average pH and total dissolved solids (TDS) concentrations of leachates from the
MBLP tests are presented in Table 3. The pH levels of the leachates generated from the
distilled water leach tests on the bottom ashes were all alkaline, and ranged from 7.81
for sample PTI2 to 11.03 for sample PT5. The pH levels of bottom ash leachates
generated using the more aggregsive le,qching media (the acidic and synthetic solutions)
were acidic, and ranged from 4.7 for sample PT5 to 5.45 for sample PTI2. Boiler and
economizer ash leachates were mildly acidic with all three types of leaching media. The
TDS results indicate that the fly ashes were much more soluble than the bottom ashes.
Results from the MBLP tests are shown i~ Fig. 5 and are expressed in terms of
leachable fractions. Leachable fraction is defined as the ratio of the mass of a metal in
lh, ary metal leachabili O" 233

TABLE 3
Average pH and total dissolved solids results for leachates from PEI-EFW
and APC pilot plant ashes

Distilled water batch


pH pH
Ash type pH TDS(mgl -~) acidic solution synthetic solution

PEI~EFW
Bottom ash 9.10 1085 5.31 5.01
Boiler ash 5.96 26,700 4.58 4.62
Economizer ash 5.92 26,500 4.75 4.76

APC pilot plant


Wets,try ash 12.00 3880 NA NA
Dry ash i 1.45 4645 NA NA
Fabric filter ash 11.55 18,850 NA NA

NA. data not available.

the leachate to the mass of that metal present in the ash sample. The results of the
distilled water leach test were used to determine the immediate leachability of the
metals in an ash (i.e. the leachability under non-aggressive leaching conditigns). The
immediate leachability of the metals in the PEI-EFW bottom ashes was very low, with
less than 0.059/o of any metal being leached. The use of more aggressive leaching media
increased heavy metal leachability significantly. Up to 6.7~ of the cadmium, 29~ of
copper, 17~ of lead, and 219/o of zinc were leached with the acidic and/or synthetic
leaching media. These increases are primarily due to the mildly acidic pH of the leaching
media. Despite the increased leachability .under the more aggressive leaching conditions,
this is not likely to pose a significant hazard to the environment because of the low
metal concentrations in the bottom ashes. This will be verified in future studies by
subjecting all types of MSW ashes io a regulatory leach test (e.g. the Government of
Ontario (1983) Regulatio n 309 Leachate Extraction Procedure). to determine their
classification as hazardous or non-hazardous wastes.
The immediate leachability of the economizer and boiler fly ashes under both non-
aggressive and aggressive leaching conditions was higher than the bottom ashes. With
the non-aggressive leaching medium, up to 1009/oof the cadmium, 63~ of the zinc, 369/o
of the copper and 0.109/o of the lead in the fly ashes were solubilized. The use of more
aggressive leaching media made little difference to the leachability of cadmium, lead
and zinc. Copper concentrations, however, increased under the more aggressive leaching
conditions with up to 609(,, of the copper present in the ashes being leached. The
difference in leachability between the bottom and fly ashes is consistent with the findings
of a recent study by the State of Washington's Department of Ecology (Knudson 1986).

5.2. Elakt pilot plant


5.2.1. Metal concentrations ht ashes
The average heavy metal concentrations in the pilot plant ashes are shown in Fig. 6.
Typically, these ashes were found to contain high concentrations of lead (up to 8300
ppm) and zinc (up to 19 000 ppm) and only r ~ d e r a t e concentrations of cadmium and
copper (up to 358 and 684 ppm, respectively). Concentrations of cadmium, lead and
234 S.E. Sawell et al.

100
,~ INCINERATOR ASH

I eo
80
40
3o

lO

Od Ou PARAMETER I'b Zn

100 . . . .

IIo

IO
o

100 ~ ~ ~ ~ tt 20:1 "

8,o

i" 4O

10
0
Od Ou
PARAMt'IXR
lib 7at

Fig. 5. Total leachability by the MBLP for the PEI-EFW ashes.

zinc were fot, nd to increase from the wet-dry scrubber ash through to tile fabric filter
ashes. This is probably due to the metals condensing out of the flue gases and adsorbing
onto the surfaces of the ash particles, which are subsequently captt, red in the pro-
gressivcly more efficient pollution control devices. Copper concentrations were similar
in all ashes.

5.2.2. hnmediate leachahility


Typical leachable fraction results for cadmium, copper, lead and zinc from the distilled
water batch leach tests are shown in Fig. 7. The results indicated that copper and lead
llear.r metal leachability 235

~ FABRIC FILTER ASH :*:.*:

I
10000 DRY -:::
SCRUBBER ASH
E
i:i:
n t7777] W ~ - D R Y
o. 8000 SCRUBBER ASH

z
o 6000 :i'i:
%%,
,,.%,
I-- %%,
%%,
n,- %%,
'o'd
I- 'o~
z 4000 'So%
.4~
bJ ,%~
to
Z
0
tO 200O ,%o,
,%o,

Cd Cu Pb Zn
PARAMETERS
Fig. 6. Average heavy metal concentrations in ashes from the Flakt pilot Plants.

100
WET-DRY DRY
80

6 o -

r 40
z
o
F- 20
o
~b_100
Cd Cu Pb Zn
LLI
~
m 8o

I
~ 60
IMMEDIATE LEACHABLE FRACTION
--J FROM BATCH LEACH TEST
4O
SHORT-TERM LEACHABLE
[~'727/2~ FRACTION (SCE:A+B)
20
LONG-TERM LEACHABLE
FRACTION (SCE:A+B+C)
Cd Cu Pb Zn

Fig. 7. Comparison of immediate, short- and long-term leachable fractions for a typical set of pilot plant ashes.

were the most immediately soluble contaminants in the ashes, especially lead from
some of the fabric filter ashes. Up to 36~ of the lead was leached by distilled water
indicating that it may have been in the form of a readily soluble chloride or hydroxide
salt. The relatively low concentrations of cadmium and zinc measured in the leachates
(up to 0.15~ of cadmium and'2.13~ of zinc) was the result of the amphoteric nature of
the metals and the alkalinity of the leachates (Fig. 7).
The pH and TDS concentrations in the leaehates from the distilled water batch leach
tests are presented in Table 3. The pit levels for all of the pilot phmt ash leachates were
highly alkaline, ranging from an average or 1 !.45 to 12.0. A plot of the ieachate pH
versus metal leachable fraction is given in Fig. 8, and ilh, strates how metal solubility
236 S.E. Sawell et al.
40

v
Z 30
0
I-.- COPPER
0 LEAD
t=_ 20 o ZINC
la.i
._1

'1-
C.~ 10
lad
,--I

0
9 10 It 12 13
pH (unlts)
Fig. 8. Metal leachability versus pll in distilled water leachates from fabric filter ashes.

remained relatively constant over the pH range 9.7 to 12.0, then increased above pH
12. Figure 8 is discussed in more detail later.

5.2.3. Short- atut long-term leachability


Results from the SCE procedure were used to estimate the short- and long-term leach-
ability of the metals in the ashes. Short-term leachability estimates indicate the potential
for metal mobility under normal landfill conditions and are based on the total of
Fractions A and B from the SCE. Long-term leachability estimates indicate the
potential for metal mobility under the more severe leaching conditions of an old landfill
site and are based on the total of Fractions A, B and C. Short-and long-term leachability
estimates arc shown in Fig. 7.
The data indicate that substantial quantities of cadmium (up to 100To), copper (up to
759/o), lead (up to 959/0) and zinc (up to 859/0) are available for leaching over the long-
term for the fly ashes from the pilot plant, especially the fabric filter ashes. The higher
leachability of the fabric filter ashes, is reflected in the higher TDS concentrations
measured in the leachates from these ashes (Table 3). The higher leachability could be
due to the formation of soluble heavy metal salts in the exhaust gas, which condense
out in the fabric filter device. It may also be due to the smaller particle size of the fabric
filter ash, as waste leachability and adsorption increases with increased surface area.

5.3. Conqmrison of PEI-EFIV and pilot phmt resuhs


5.3.1. Metal concentrations in ashes
In general, copper concentrations in the fly ashes from both facilities were similar (Figs
4 & 6). However, ashes from tile pilot plant contained only a fraction (10-30~) of the
cadmium, lead and zinc concentrations found in the PEI-EFW ashes. Such a large
difference may be due to several factors: (!) concentrations of heavy metals in the
exhaust gas are dependent upon the refuse content which is highly variable, especially
between different municipalities; (2) the low metal concentrations in the pilot plant
ashes were partially due to the addition of li'~e to the gas stream which increased the
final mass of the ash; and (3) the difference in process operating conditions (e.g. burn
lteavy metal leachabiliO. 237

temperature, excess air addition, recycle rate, etc.) could have affected the heavy metal
concentrations.

5.3.2. hmnediate leachabilio'


hnmediate leachable fraction results for cadmium, copper and zinc from the PEI-EFW
fly ashes were much greater than those from the pilot plant ashes. The difference appears
to be due to metal speciation and metal solubility dependence on pH. In general, tile
heavy metals were probably speciated as hydroxides or chlorides, which are amphoteric
in nature and are, therefore, more soluble under acidic or highly alkaline conditions
than under neutral or mildly alkaline conditions. The slightly acidic pH levels which
predominated in the PEI-EFW fly ashes resulted in increased metal solubilization. The
acid levels may have been due to HCI in the flue gas, sorbing onto particulates. Con-
versely, the lower metal solubilities from the APC fly ashes were probably due to the
alkaline pH levels of the ash caused by the lime addition to the flue gas stream.
The leachability results for lead show a different trend. Lead in the PEI-EFW fly
ashes remained insoluble even under mildly acidic conditions while lead solubility in
the pilot plant ashes increased with increasing alkalinity (Fig. 8). The results for the
pilot plant ashes are consistent with solubility curves for lead in the pH range from 9 to
13 (C6t6 1986); however, the rcason for the low concentrations measured in the leach-
ates from the PEI-EFW ashes, especially with the very high concentrations present in
the ash, is not known. It is possible that the lead was present as an insoluble sulphide
or silicate in the PEI-EFW ashes. Subsequent ash characterization studies should in-
clude the use of X-ray diffraction or scanning electron microscope techniques to identify
d.ifferent metal species which would help in estimating heavy metal leachability.
The short-term leachable fraction results for the pilot plant ashes are comparable to
the immediate leachable fraction results for the PEI-EFW fly ashes. This suggests that
the lime addition to the flue gas stream in the APC system provides only a limited
buffering capacity to the ashes, and that significant quantities of heavy metals in the
ashes are potentially available for leaching under normal landfill conditions.

6. Conclusions
The results indicate that MSW bottom ashes are relatively insoluble and may be
considered suitable for landfilling. MSW incinerator boiler and economizer fly ashes,
on the other hand, contain high concentrations of heavy metals, especially lead and
zinc, which are readily available for leaching under normal landfill conditions. Even the
addition of lime to the flue-gas stream in the APC system provided only a limited
buffering capacity to the ashes. Contaminant leachability from these ashes appears to
be dependent upon several factors, including combustion temperature, the pH of the
resultant ash, ash particle size, and metal speciation.

7. Recommendations
The results obtained here and-in othel- preliminary studies, such as that by Knudson
(1986), indicate that MSW incinerator fly ash residues may require treatment (e.g.
solidification, vitrification, metal recovery, etc.) prior to landfilling.
Further ash characterization studies are required to identify the potential mobility of
a wide range of contaminants in ashes from ~ wide range of EFW facilities. Research
and development of stabilization techniques for these residues is also warranted.
238 S.E. Sawell et al.

To fulfil these requirements, Environment Canada, under N I T E P , and the U.S.


Environmental Protection Agency, are presently co-ordinating their experimental
programs in the field of MSW incineration. Future co-operative efforts will concentrate
on increasing our understanding of the effect of incinerator operating conditions on the
leachability of MSW ashes.

References
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leachability from solid wastes, lVater Scienbe Technology, 19, 1029-1036.
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Environment Canada (1986), The national incinerator testing and evaluation program: air
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Phung, H. T., Lund, L. J., Page, A. L. & Bradford, G. R. (1979), Trace elements in fly asia and
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