Professional Documents
Culture Documents
DOI 10.1007/s12649-016-9551-z
ORIGINAL PAPER
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Waste Biomass Valor
any treatment or acceptance test for the production of source of carbon dioxide- for use in the controlled accel-
cement, bricks and expanded clay; (2) for road construction erated carbonation of the BA produced by the incineration
or environmental restorations if leaching test results com- plant itself. Differently from previous works [12],—we
ply with limits reported in the following in Table 2. investigated accelerated carbonation reaction, by experi-
Leaching tests must be performed according to the UNI mental set-up, using simulated flue gases of incinerators,
10802 and methods reported in UNI EN 12457-2. The first assuming a volumetric content of CO2 equal to 10–12 %
option—production of cement, bricks and expanded clay— [12, 17].
should be encouraged, being applicable without any treat- We applied accelerated carbonation of BA following the
ment or acceptance test and hence simpler than the other direct carbonation route, through a direct gas/solid contact.
one. However, methods for making possible the application The CO2-containing gas flows through the BA fixed bed.
of the second option—use of BA in road construction or CO2 quickly reacts with readily reactive Ca-oxide phases
environmental restorations—should be investigated to (e.g. Ca(OH)2) contained in the BA, as it is summarized in
widen the potential for BA recycling. the reaction 1:
According to the Decree of the Environmental Ministry CaðOH Þ2 ðsÞ þ CO2 ðgÞ ! CaCO3 ðsÞ þ H2 O ð1Þ
dated 27/09/2010, complying with EU directives, the cri-
teria of waste acceptance in different types of landfills are CO2 is thus fixed in solid and stable form of carbonate.
defined (i.e. landfills for inert, non-hazardous or hazardous Hence, the additional environmental benefit targeted by
waste). In particular, waste can be accepted in landfills for this process is the reduction of flue gas CO2 emissions,
inert waste if the results of leaching tests, executed even if this is a very small reduction contribution with
according to the UNI 10802, comply with the limits respect to the overall emissions from the incineration
reported in Table 2. plant—Rendek et al., estimated a CO2 emission reduction
One possibility of processing this type of waste, for of 0.5–1 % [12]—as it will be illustrated in the results
making it suitable for use in civil engineering applications section, too.
or for safer final disposal to landfills, is applying stabi- The aim of the work is to preliminary evaluate if this type
lization by accelerated carbonation, with the aim of pro- of process—hypothetically built at the incineration plant
ducing a chemically stable material with improved site—can be sustainable from the economic point of view of
leaching behavior [8–12]. the company managing the incineration plant. We first car-
Accelerated carbonation may be applied following the ried out a preliminary laboratory investigation using a sim-
indirect route—by which the alkaline metals are first ulated flue gas with CO2 volumetric content equal to 10 %,
extracted from the silicate matrix and then precipitated as since, to the best authors’ knowledge, no data are available in
carbonate—or the direct carbonation route, by which the literature about BA carbonation test using stream at these
reaction occurs either in the aqueous phase or at the gas– conditions. This preliminary laboratory investigation was
solid interface. In this latter case, predominantly, a high mainly aimed at estimating the process parameters required
purity carbon dioxide gas is used, which is expensive to for the following economic analysis (mainly the required flue
produce and buy. An alternative supply of lower purity gas volume to process a unit mass of bottom ash, which
carbon dioxide can be obtained from industrial point source influences the duration of the process and hence the size of
emissions: some authors used biogas or landfill gas for such the plant). Then, a first draft of process sizing at industrial
a process, also with the aim of reducing the CO2 content scale was performed, with the aim of evaluating the cost of
and increasing the methane one [13–16]. Bobicki et al. [17] the treatment. The estimated treatment cost might be com-
reviewed several alkaline industrial wastes that can be used pared with the costs the companies generally incur for the
for mineral carbon sequestration and the available process external treatment/disposal of BA. The objective is to supply
routes, suggesting that BA is a good candidate also thanks an initial basis for further investigation on the overall fea-
to the proximity in which the residue and CO2 in the flue sibility of the process.
gases are generated. As a matter of fact, Rendek et al. [12]
already proposed that BA may be used to capture and store
CO2 contained in industrial emission and at the same time Materials and Methods
realizing a pre-treatment stage prior to either recycling or
landfilling of BA. However, they first investigated accel- Experimental Facility
erated carbonation reaction only using pure CO2, with the
objective to understand what the possibilities and the lim- The experimental facility mainly consists of the BA fixed
itations are in view of possible technical application. bed reactor, used to realize the direct contact between the
In this study we evaluated the possibility of using the BA and the simulated incineration flue gas, and the mea-
flue gases from waste incineration plant as an alternative suring systems.
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Waste Biomass Valor
The BA fixed bed reactor is realized by a 15 l stainless able to work in the range from -100 to ?100 mbar relative
steel cylindrical container (diameter 28 cm; height 35 cm) to the atmospheric pressure with accuracy of ±0.5 % f.s. at
(Fig. 1a). The reactor can be opened from the top, by 20 °C.
means of a cover, for loading and unloading the BA. The Atmospheric pressure is measured by means of a baro-
gas flows into the filter bed from the bottom to the top. The metric pressure transducer (Delta Ohm HD 9908 BARO)
ashes rest on a gravel layer covered by a geotextile fabric, able to work in the range from 700 to 1100 mbar, with
which retains the small particles and allows the passage of accuracy of ±0.5 mbar at 20 °C and resolution 1 mbar.
the gas (Fig. 1b). For external thermal insulation, an The inlet/outlet gas temperature and the temperature
insulating adhesive material, provided in rolls, was used inside the reactor are measured by electronic thermome-
(not shown in Fig. 1a). ters, produced by Hanna Instruments (HI 98501—Check-
Input and output gas flow rates to/from the BA fixed bed temp C), able to measure in the range from -50 to
reactor are measured by means of CKD-small size flow ?150 °C with precision of ±0.3 °C and resolution 0.1 °C.
sensors FSM2-NVF010-S063, able to measure in the range The gas flow rate, pressure and temperature are mea-
0–1000 ml/min with accuracy of ±3 % f.s. and repeata- sured at sampling rate of 1 kHz, the average of the mea-
bility \±1 % f.s. sured values is registered in a discontinuous manner (every
The differential pressure of the input and output gas second). The measurement instruments are controlled by a
streams to/from the reactor is measured by a differential programmable automation controller NI-USB 6008
piezoresistive pressure transducer (Delta Ohm-HD 408T) National Instruments with 8 analog inputs (12-bit, 10 kS/s);
2 analog outputs (12 bit, 150 S/s); 12 I/O digital; 1 counter
32 bit; programming software Labview 10.0.
Besides, the experimental facility is equipped with a gas
mixing device (Witt MG 100-3ME EEx), able to produce
CO2/N2 gas mixtures of different compositions. The device
allows setting the desired volumetric concentration for 5 %
steps with an accuracy of ±2 % abs.
Materials
Experimental Tests
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Waste Biomass Valor
the BA behavior with respect to the reaction with CO2 [12]. studies concerned with different types of applications [15].
N2 does not react with BA, thus the difference between the After finishing the test, a BA sample was collected for each
inlet and outlet flow represents the CO2 subtracted by the test.
carbonation reaction. BA samples were analyzed before and after the treat-
The amount of captured CO2 can be estimated from the ment with respect to the leaching behavior of metals by an
difference between the entering and the exiting volume of external laboratory, according to methods acknowledged
gas, at a given time of the experiment, since the captured by Italian technical legislation. Leaching tests were per-
gas is only CO2, by using Eq. 2: formed according to the UNI 10802 and methods reported
in UNI EN 12457-2, applying one stage batch test at a
Vin;t Vout;t
CO2;captured ¼ MCO2 ð2Þ liquid to solid ratio of 10 l/kg, using deionized water. The
Vm
analysis of the eluates was performed according to UNI EN
where CO2,captured is the mass of captured CO2 (in kg) at a 16192:2012 to determine the metals contents.
given time t; Vin,t is the volume of gas flowed in at time t Results were compared with limits for reutilization and
(reported at normal conditions of pressure = 101325 Pa landfill for inert waste, as set by the Italian regulation cited
and temperature = 273 K; expressed in Nm3); Vout,t is the before.
volume of gas flowed out at time t (expressed in Nm3); Vm Average BA measured humidity was 25 % in mass. The
is the volume of one kmol of ideal gas at normal condition tests were conducted at room temperature with average
(equal to 22.414 Nm3/kmol); MCO2 is the CO2 molar value of 20 °C. An average increase of 4 °C was registered
weight (equal to 44 kg/kmol). during the tests. The tests prolonged for more than 60 h,
The experiment was repeated at the same conditions for thus they were stopped—closing the inlet flow and the
three times. The required BA amount for the three tests was reactors—during night time and started again in the fol-
prepared starting from about 30 kg of BA, after appropriate lowing morning.
homogenization and removing the large metal particles and
in general large aggregates. No systematic sieving was Preliminary Experimental Results
carried out at this time. A sample from each of the prepared
amount was collected before filling the reactor. The Table 1 reports the results of the leaching tests carried out
amount of BA loaded in the reactor for each test was 5 kg, for the BA before and after their treatment.
while the inlet flow rate was set at 20 Nl/h, realizing a From the results of the leaching test of the BA sampled
specific flow rate equal to 4 Nl/(kg h), as a first approach before the treatment—reported in Table 1—one can
value, which was found as appropriate from previous understand why a treatment is required before reusing or
Table 1 Results of leaching tests for samples of BA before and after the carbonation treatment, compared with regulation limits for reuse and
disposal in landfills for inert waste
Metal Limits for reuse* Limits for landfill of inert waste** Non-processed BA Processed BA Units
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Waste Biomass Valor
disposing the BA to inert landfills. In particular the sam- The volume of the gas entered and exited to/from the BA
pled BA exhibited leaching values exceeding the limits for reactor at the end of the test is reported in Table 2, together
reuse or inert landfills in relation to lead. The leaching with the calculated amount of captured CO2 and the specific
value of barium was lower than the acceptance limit for BA uptake. The average inlet flow rate was 21.42 Nl/h,
inert landfilling but very close to it, and it was higher than slightly higher than the target value of 20 Nl/h. About 1285
the limit for reuse. The leaching value of zinc was lower Nl of simulated flue gas flowed through the 5 kg of BA
than the limit for inert landfilling, but very close to it. The fixed bed, thus about 257 Nl were used to process 1 kg of
leaching value of copper exceeded both the limits for reuse BA, according to these experimental tests. As reported in
or inert landfills. Table 2, about 37 g of CO2 are captured per each t of BA.
Figure 2 shows the trends of the inlet gas flow rate (Qin) Considering that from the incineration of 1 kg of residual
and the outlet gas flow rate (Qout), respectively to and from municipal solid waste, originated about 0.2 kg of BA, the
the BA fixed bed reactor as average values of the repeated captured CO2 would be about 7.4 g per each kg of MSW. If
tests, together with the average values of the percent dif- we consider that residual municipal solid waste non-re-
ference between the inlet and outlet flow. newable carbon content is about 0.1–0.15 kg/kg, we obtain
As it can be noticed from Fig. 2, the CO2 in the inlet flow a production of about 0.37–0.55 kg of CO2 per each kg of
is captured by the BA, thus the gas exiting flow is always waste. The CO2 captured by BA carbonation represents
lower than the entering one. For more than two thirds of the about 1–2 % of total non-renewable CO2 produced by the
test duration, the percent difference between the inlet and combustion, in accordance with literature [12].
outlet flow is higher than 7 %, i.e. more than 7 % of the inlet The results in Table 1 show that the carbonated BA has
CO2 is captured. In the last part of the test the percent dif- a lower leaching for lead, barium and zinc. The lead
ference starts to decrease at values lower than 5 %, showing leaching is substantially improved, being reduced to values
that the BA carbonation ability is depleting. When the per- lower than the limits for reuse or inert landfills. The initial
cent difference remained below 4 % for few hours, it was value of barium was very close to the acceptance limit for
decided to stop the tests, even if the carbonation activity inert landfilling, but higher than the limit for reuse: after
might continue slowly for additional time. The overall carbonation also this second limit is complied. The zinc
average time duration of the tests was about 60 h. content already complied with the limit for reuse and was
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Waste Biomass Valor
very close to the limit for inert landfilling: after carbona- Industrial Scale Plant Sizing and Economic
tion the leaching value was substantially reduced. Evaluation
Reduction in leaching of lead (lowering of about two
orders of magnitude) and zinc (lowering of about one order Even if the results about the copper and antimony leaching
of magnitude) thanks to BA carbonation treatment is posed some criticisms about the possibility of changing the
extensively reported in the scientific literature [4, 11, 12, classification of BA from non-hazardous waste to inert
19, 20]. Similarly, barium leaching reduction after BA waste or recoverable waste, a preliminary assessment of the
carbonation is reported by several authors [10, 11, 21]. process from the economic point of view was performed, to
On the other side, the carbonated BA shows an increase estimate if it is worth to investigate more in deep the
in the leaching of: nickel, vanadium, chromium, molyb- behaviour of different size range particle of BA in this
denum, antimony and copper. specific application. The preliminary results obtained from
However, concerning nickel, vanadium, chromium and the experimental set-up were used for carrying out a draft
molybdenum both the non-carbonated and carbonated BA sizing of the process on industrial scale in order to further
presents leaching metal concentrations lower than limits estimate the treatment cost.
for reuse or inert landfills.
Antimony leaching value was below inert landfill limit Industrial Scale Plant Sizing
(no limits for reuse), but it increased over such limit after
the carbonation process. This increasing behavior is in The reference incineration plant was assumed to burn about
agreement with what reported by other authors [10]. 70,000 t/y of MSW producing about 14,000 t/y of BA, as
Copper leaching concentrations were above the limits the 20 % in mass of entering waste. It is assumed to extract
for reuse and inert landfill even before carbonation process part of the exhausted gases flow rate at the stack—so after
and further worsen after carbonation process. Such wors- the flue gas treatment—and convey them through the BA
ening is in agreement with other results [11], reporting that carbonation reactor. Exhausted gas temperature at the stack
copper is generally the only metal that is not reduced below is about 120 °C, however, during the path to the reactor the
reuse limits. gases cool down and it is possible to assume that the
For the other metals (beryllium, cobalt, arsenic, cad- temperature will be not far from the ambient one. Overall
mium, selenium and mercury) the leaching concentration exhausts flow rate is around 50,000–60,000 Nm3/h.
was below the detection limit for both the carbonated and Concerning the carbonation reactor, it was assumed to
non-carbonated samples and in any case far below the inert use a reactor technology that was originally proposed for
landfill or reuse limits. the composting or the aerobic biostabilization of
In summary, it is possible to state that the carbonation biodegradable waste, based on the use of industrial con-
process had a positive effect on lead and barium decreasing tainers (Fig. 3a). The system is, indeed, already equipped
the leaching concentration below the reuse/inert landfills with an air insufflation system—in our case substituted by
limits and a negative effect on copper and antimony, flue gases insufflation system—and a leachate collection
increasing the leaching concentrations which did not system due to its original function. This technology offers
comply with the considered limits. As a matter of fact, substantial advantages, mainly related to the modularity of
before carbonation process the BA presented leaching the treatment, which makes it suitable for different plant
concentrations not suitable for inert landfills/reuse for lead, sizes, and to the simplification of the movement operations,
barium and copper, while after the carbonation process the since each container can be moved by a truck. In this way,
BA showed leaching concentrations suitable for reuse the empty container is brought by the truck in the loading
except for copper (antimony is not regulated) and suit- area where BA is loaded by a conveyor belt by the top of
able for inert landfill except for copper and antimony. It is the container. The container, containing exhausted BA
likely that heavy metals are mainly present into the fine after the treatment, can be unloaded by the truck in the
fraction of BA, namely with size lower than 2–5 mm [10, appropriate storing area (Fig. 3b).
22]. Thus additional investigations of the behavior of the Each container has a volume of about 25 m3 (length
different size range particles should be carried out in future 6.5 m, width 2.5 m, height 2.65 m). We considered here to
to ascertain if it is possible to improve the behavior of such use only 20 m3 of the available volume, to account for the
fine fraction or alternatively just separating the fine fraction higher specific weight of BA with respect to biodegradable
by sieving and sending it to safe disposal. waste. Thus assuming a specific weight of 1.7 t/m3 for the
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Waste Biomass Valor
Economic Evaluation
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Waste Biomass Valor
Table 3 Main sizing parameters of the process on industrial scale during our experimental tests—and the different exhausted
gas flow rates.
t Day 4 6 9
We also considered that moisture accumulation at the
mBA,day t/day 68 68 68 bottom of the reactor is likely, both due to the BA and
mcontainer t 34 34 34 exhausts humidity. The cost for the external appropriate
nactive 8 12 18 treatment of such leachate, originated from the exhausts
n 9 13 19 humidity, was preliminarily accounted for, assuming 15 %
3
Qspec Nm /(htBA) 4 4 4 in volume of water in the exhausts—assuming precau-
Qfluegas Nm3/h 1088 1632 2448 tionary the complete condensation—and a specific cost of
treatment equal to 23 €/m3 of leachate.
A summary of the utilities consumption (electricity and
diesel), leachate production and operating costs is reported
required compressor power was estimated assuming a in Table 5.
specific pressure loss experienced by the exhausted gas The most important contribution to the capital costs is
through the BA layer equal to 0.9 mbar/cm—estimated due to the reactors (69–78 %) and the truck for BA
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Waste Biomass Valor
Table 4 Summary of investment costs for the considered BA treat- If the processed BA is suitable for reuse, the revenue
ment process, for the three cases of process duration from its selling should be accounted for and it was assumed
Duration (day) 4 6 9 equal to 3 €/t [15]. If the processed BA is not suitable for
reuse, it might be suitable for inert landfill disposal; in this
Container system (Euro) 381,893 482,028 616,280
case the additional cost for the disposal needs to be added
Truck (Euro) 172,500 172,500 172,500 to the STC and it was assumed equal to 10 €/t [25]. To
Compressor (Euro) 1908 3123 5078 account for the uncertainty of the complete success of the
Conveyor belt (Euro) 4869 4869 4869 treatment (previously highlighted problems with copper
Piping (Euro) 14,029 16,563 19,968 and antimony) we also considered that if the processed BA
Total investment (Euro) 556,301 657,651 793,858 is neither suitable for inert landfill disposal, it needs to be
disposed off in landfills for non-hazardous waste (i.e. the
applied process was not useful), accounting for an addi-
Table 5 Summary of utilities consumption, leachate production and tional cost of 70 €/t.
O&M costs (€/y) The final cost (FC) incurred for the management of BA
may be calculated by Eq. (7), depending on the percentage
Duration (day) 4 6 9
of processed BA that can be sold for reuse (R) and the
Diesel consumption (l/y) 3090 3090 3090 percentage of BA that can be disposed off in landfill for
Electricity consumption (kWh/y) 29,876 44,708 64,484 inert waste (IW):
Leachate production (m3/y) 648 972 1458
FC ¼ STC þ ðIW IW RÞ Cinert þ ð1 IW Þ
Annual amortization (Euro/y) 75,583 89,354 107,860
Cnonhazardous IW R Csold ð7Þ
Maintenance (Euro/y) 19,471 23,018 27,785
Personnel (Euro/y) 100,000 100,000 100,000 where Csold is the specific cost at which BA is sold for
Diesel (Euro/y) 4295 4295 4295 reuse; Cinert is the disposal cost in landfills for inert waste;
Electricity (Euro/y) 4780 7153 10,317 Cnon-hazardous is the disposal cost in landfills for non-haz-
Leachate treatment (Euro/y) 14,904 22,356 33,534 ardous waste and SPT is assumed equal to 20 €/t (the worst
Total annual cost (Euro/y) 219,033 246,176 283,791 case previously calculated and reported in Table 5). The
Specific treatment cost (Euro/t) 16 18 20 trend of the FC versus the IW percentage, for R corre-
sponding to 0 and 100 %, is shown in Fig. 5.
The last row reports the calculated specific treatment cost
When the percentage of sold BA is zero, the final cost—
i.e. treatment cost plus disposal in inert landfill—is lower
than the direct disposal cost of un-treated BA equal to
movement (22–31 %). Annual amortization of the capital 70 €/t, if the percentage of BA disposed in inert landfill is
cost represents about 35–38 % of the annual cost. The most higher than about 34 %.
relevant contribution among the operating costs is repre- While for increasing percentage of sold BA, the FC
sented by the labour (35–46 %). decreases and becomes lower than the treatment cost and
From the total annual cost, dividing by the total annual equal to 16 €/t, in case of the possibility to sell the 100 %
amount of processed BA (i.e. 14,000 t), it is possible to of treated BA.
calculate the specific treatment cost (STC) for a unit of The final cost of the process remains at values lower
mass of BA, as reported in the last raw of Table 5. The than the reference cost for non-hazardous landfill, even if
STC ranges from 16 to 20 € per t of BA. part of the carbonated BA is not suitable neither for reuse
or inert landfilling. This observation leaves open the pos-
sibility to preliminary sieve the BA and eventually to dis-
Discussion pose off, in non-hazardous waste landfills, the fractions for
which it is not possible to improve the leaching behaviour
As anticipated BA is generally disposed off in landfills for of some metals, likely copper and antimony.
non-hazardous waste at a specific cost of ranging from
about 45 €/t in Austrian case [24] to 70 €/t or even more in
the Italian case [15, 25]. Conclusions
With reference to the prosed process, after the carbon-
ation, the BA may be disposed off in a landfill for inert The final disposal or reuse of bottom ash from waste
waste or reused in construction works, if the metal leaching incineration is strictly linked to the potential release of
accomplishes the limits highlighted before (assuming that constituent contaminants into the environment. One pos-
also criticism about copper and antimony can be resolved). sibility of processing this type of waste, for making it
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Waste Biomass Valor
suitable for use in civil engineering applications or for safer 6. ISPRA: Rapporto Rifiuti Urbani 2012. Rapporto 163/2012. www.
final disposal to landfills, is applying stabilization by isprambiente.gov.it (2012)
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