Waste Management 22 (2002) 951–955

www.elsevier.com/locate/wasman

Treatment of industrial landfill leachate by means of

evaporation and reverse osmosis
Luca Di Palma*, Paola Ferrantelli, Carlo Merli, Elisabetta Petrucci
Dipartimento di Ingegneria Chimica, dei Materiali, delle Materie Prime e Metallurgia, Università di Roma ‘‘La Sapienza’’, Via Eudossiana,
18-00184 Roma, Italy

Accepted 13 June 2002

Abstract
In this paper a process for the treatment of landfill leachate involving evaporation and reverse osmosis was proposed. Experi-
mental tests were performed on an industrial landfill leachate. The leachate was subjected to evaporation so as to obtain a distillate
containing a small amount of organic material and a substantial amount of inorganic substances (consisting primarily of metals and
ammonium salts). The distillate of the evaporation treatment was then subjected to reverse osmosis. The reverse osmosis tests were
performed using two different membranes: the AD membrane (thin two-ply film of polyamide) and the SC membrane (thin three-
ply film of polyamide). Tests carried out at different values of pH showed a reduction of organic content of about 88% when AD
membranes were used and about 80% with SC membranes independently of pH. As regards ammonium, comparable reductions of
over 97% were registered for both types of membrane in the optimal conditions of pH=6.4 (97.1% for AD membranes and 97.7%
for SC).
# 2002 Elsevier Science Ltd. All rights reserved.

1. Introduction volumetric flow, the generally adopted treatment deals

Controlled dumping is regarded as an efficient, eco-
nomical and technically sound system of disposal for
solid waste. The release from a landfill consist mainly of
methane gas, that is a resource which can be utilized for
energy production, and leachate which has became the
subject of recent interest as a strongly polluted waste
water. Over the years, management of this system has
led to important innovations in landfill technology
designed to limit its potentially negative impact on the
environment. The need to reduce the risk of the
uncontrolled dispersal of landfill leachate in the envir-
onment forms part of the general criteria involved in
landfill design. In any case, it is essential to provide for
systems of leachate drainage and treatment. Because of
landfill leachate is a complex wastewater with
considerable variations in both composition and
* Corresponding author. Tel.: +39-06-44585571; fax: +39-06-
44585622.
E-mail address: luca.di.palma@ingchim.ing.uniroma1.it (L. Di
Palma).
0956-053X/02/$ - see front matter # 2002 Elsevier Science Ltd. All rights reserved.
PII: S0956-053X(02)00079-X
on a series of different step.
Reverse osmosis (RO) (Lonsdale and Podall, 1972;
Sourirayan, 1970) usually constitutes the last stage of a
process that may consist of biological treatment (Chian
and Dewalle, 1976), coagulation-flocculation treatment
(Amokrane et al., 1997; Slater et al., 1983), or other
membrane treatment (ultrafiltration, microfiltration)
(Baker, 2000; Sysdek and Ahlerts, 1984).
Several studies were performed, both at lab and
industrial scale, to investigate RO performances on the
separation of pollutants from landfill leachate (Krug
and McDougall, 1989; Linde et al., 1995; Bilstad and
Madland, 1992; Kinman and Nutini, 1991). In recent
years the feasibility of using RO technologies for
municipal leachate disposal with low organic content
was assessed (Chianese et al., 1999). In the case of
industrial landfill leachate the contemporaneous
presence of both high concentration of organic
compounds, ammonia and heavy metals strongly affects
treatment performances.
In this paper a process for the treatment of an indus-
trial landfill leachate with high organic and ammonia
content by means of evaporation in vacuum conditions
952 L. Di Palma et al. / Waste Management 22 (2002) 951–955

followed by reverse osmosis was proposed. The main
aim of the evaporation stage was to concentrate
ammonia, heavy metals and organic compounds, in
order to reduce water flow and increase RO stage
efficiencies. The operative conditions to obtain a satis-
factory reduction of the volume of leachate together
with a suitable concentration of the distillate for the
subsequent stage of reverse osmosis were so optimized.
In order to reduce energy consumption the possibility of
using a service fluid already available at temperatures of
35–40
C for heating (thus reducing energy consump-
tion) was evaluated.
RO tests were then performed at different pH in order
to grant complete ammonia removal.
2. Experimental
Three series of evaporation tests were performed at
T=40
C. Operative pressures were respectively 400
mmHg, 45 mmHg and 20 mmHg. The cooling water
temperature was 15
C. The distillate obtained in the
tests performed at 45 mmHg was collected and sub-
jected to the RO treatment.
The RO tests was carried out at room temperature in
Berghoff GH 100 cells fitted with flat polyamide mem-
branes (with a surface area of 0.0044 m2). Polyamide
membrane ensure in fact a high rejection in a wide pH
range (Baker, 2000).
Two types of Desal membranes were used in the
process:
 AD (thin two-ply film of polyamide)
 SC (thin three-ply film of polyamide).

Table 1 gives details of the characteristics of the
leachate used in the experiments. The high organic and
ammonia content suggested to perform an evaporation
step before RO treatment, in order to avoid membrane
fouling.
2.1. Procedure
The experimental tests were performed on 250 ml
samples. Evaporation tests were carried out in a Büchi
R-114 vertical rotating evaporator connected to a KNF
N 819 vacuum pump. In order to ensure a good mixing
and to avoid scaling, the chosen operative rotational
speed was 10 rpm.
In preliminary tests the selected membranes were tes-
ted in order to assess their efficiency in salts removal.
These tests on a 3 wt.% NaCl aqueous solution were
performed. Membrane rejection in the range between 30
and 90 bar and in the polyamide membranes optimal
pH range at P=60 bar was determined. Solute rejection
was evaluated in term of conductivity.
Tests on the evaporation distillate was finally per-
formed in the range of pH between 6 and 10 after acid-
ification with an H2SO4 96 vol.% solution, in order to
determined the optimal conditions for ammonia
separation.
Solute rejection was calculated as:
cp
R¼1 ð1Þ
cf

Table 1
Characteristics of the leachate used in the experimentation
where cf and cp are the solute (TOC or ammonia) con-
centration on the feed and on the permeate respectively.
Parameter Unit Value

COD mg/l 19,900 2.2. Chemical analyses

BOD5 mg/l 4000
TOC mg/l 5244 COD was determined according to standard methods
Conductivity mS/cm 79,800 (APHA–AWWA–WEF, 1989). pH was measured with a
pH – 8
Density kg/dm3 10,552
Crison 421 pH meter. Total organic carbon was deter-
Na+ meq/l 1012 mined using a Shimadzu TOC-5000A TOC Analyzer.
K+ meq/l 39.6 Ionic species concentration was determined by means
Mg2+ meq/l 186.3 of ionic chromatography using Dionex DX 120 equip-
Ca2+ meq/l 1.08 ment. Metals concentration was measured by means of
Ba2+ meq/l 3.43
NH+ meq/l 217.6
a Philips PU 9200 atomic absorption spectrophotometer.
4
F meq/l 10.07
Cl meq/l 1293
Br meq/l 0.71 3. Results and discussion
SO=4 meq/l 6.05
Cu2+ meq/l 0.032
Cr3+ meq/l 0.013
3.1. Evaporation
Fe3+ meq/l 0.18
Pb2+ meq/l 0.02 Preliminary tests were carried out at P=400 mmHg
T=40
C on 250 ml samples. In these conditions,
 L. Di Palma et al. / Waste Management 22 (2002) 951–955 953

Fig. 1. Volume and TOC of distillate as a function of time (P=400 Fig. 3. Volume and TOC of distillate as a function of time (P=20
mmHg). mmHg).

Table 2
Characteristics of the evaporation distillate and residue

Parameter Unit Residue Distillate

COD mg/l 78,000 200.5

TOC mg/l 20,640 53.1
Na+ meq/l 5783 0.18
K+ meq/l 121 –
Ca2+ meq/l 58 –
NH+ 4 meq/l 733 33
F meq/l 45 0.3
Cl meq/l 5550 28
Br meq/l 2 –
SO=4 meq/l 4 0.04
Cu2+ meq/l 0.25 –
Fig. 2. Volume and TOC of distillate as a function of time (P=45 Cr3+ meq/l 1.4 –
mmHg). Fe3+ meq/l 4.25 –
Pb2+ meq/l 0.08 –

evaporation took place slowly. Fig. 1 shows that three

different phases in the process were observed.
Due to the fast stripping of volatile organic
compounds, a low volume of distillate with high TOC
values was collected. The following solvent evaporation
caused the increase of collected distillate volume. As a
result of this dilution, the organic content in the
distillate decreased, reaching its lowest value in corre-
spondence of a distillate collected volume of 75%.
Following the evaporation of heavier organic com-
pounds a new increase in TOC concentration was then
observed.
Fig. 2 and 3 show the experimental results of the tests
performed at the same temperature, but at 45 and 20
mmHg respectively.
In these tests carried out at higher degrees of vacuum,
the first two phases previously observed in the evapora-
tion pathways took place simultaneously.
When the collected volume of distillate was about 70–
75% of the initial sample, a TOC value of about 70 mg/l
was observed.
The complete removal of the inorganic fraction and of
the residual amount of organics was then left to the
subsequent phase of membrane treatment.
In the tests performed at 45 mmHg, 70% of sample
recovery in the distillate was observed after 50–60 min.
At a higher degree of vacuum (20 mmHg), it took only a
few minutes less to achieve the same results.
A pressure of 45 mmHg was therefore regarded as
optimal for the evaporation treatment at the selected
operative temperature.
The characteristics of the distillate and the residue
obtained are shown in Table 2. The pH of the evapora-
tion distillate was about 9.5.
Results show that the evaporation stage can success-
fully strongly reduce the organic and ammonia level in
the solution. In addition no significant metal con-
centration in the permeate was observed. This allowed
the following membrane stage operate with higher flows
and reduce fouling compounds concentration.
3.2. Reverse osmosis
The distillate obtained in the tests performed at 40
C
and 45 mmHg was then subjected to the reverse osmosis
tests.
954 L. Di Palma et al. / Waste Management 22 (2002) 951–955
Figs. 4–6 show that increasing the operative pressure
in the investigated range, the membrane rejection
increased, while the maximum rejection in the pH range
between 5 and 8 was observed. The maximum flow rates
in the investigated pressure range at P=60 bar was
Fig. 4. Solute rejection of the AD and SC membrane as a function of
pressure (solution of NaCl 3%).
Fig. 5. Rejection of the AD membrane as a function of the pH of the
distillate.
Fig. 6. Rejection of the SC membrane as a function of the pH of the
distillate.
observed. In these conditions the average flow was 20.2 l/
S2 h for AD membrane and 30 l/S2 h for SC membrane.
Basing on this preliminary results an operative
pressure of 60 bar was adopted for following tests.
Fig. 7 and 8 show the TOC and ammonia rejection,
R, in the investigated pressure range.
No clear difference emerged between the two types of
membrane due to the low solute content in the eva-
poration distillate that limited fouling phenomena.
A more constant flow using the SC membrane was
registered: this was probably due to the smoother
surface of SC membrane with respect to AD membrane,
and the consequent lower fouling.
pH variations in the feed solution proved to have no
effect on the reduction of the organic fraction but
showed a considerable impact on ammonium reduction.
Table 3 shows the data for the permeate at pH=6.4,
the value at which the highest reduction of the ammo-
nium ion was registered.
The obtained results lead to the following considerations:
Fig. 7. Percentage reduction of TOC and ammonium with the AD
membrane.
Fig. 8. Percentage reduction of TOC and ammonium with the SC
membrane.
 L. Di Palma et al. / Waste Management 22 (2002) 951–955 955

Table 3 This distillate was then subjected to a treatment of

Characteristics of RO permeates (P=60 bar) reverse osmosis, resulting in a further 90% reduction of
Parameter Unit Membrane AD Membrane SC its organic content. As regards ammonium, reductions
(pH=6.4; =20.7 l/m2h) (pH =6.4; =29 l/m2h) of over 97% were obtained at pH=6.4.
With respect to other alternative treatments, the pro-
COD mg/l 18 30.5
TOC mg/l 5.13 10.3 posed system displays limited environmental impact and
Na+ meq/l 0.045 0.108 a high degree of flexibility due to modular use of the
NH+ 4 meq/l 0.86 0.71 reverse osmosis unit.
F meq/l 0.02 0.024
Cl meq/l 0.6 0.76
SO=4 meq/l 0.12 0.21
References

 AD membrane shows a higher TOC rejection;
 no substantial difference between AD and SC
membrane in NH+ 4 rejection was observed;
 as would expected pH strongly affects membrane
rejection: an ammonia reduction of more than
97% at pH=6.4 was observed for both mem-
brane AD and SC.
4. Conclusions
The process of evaporation and reverse osmosis
resulted in the complete removal of the pollutants con-
tained in an industrial landfill leachate.
The evaporation tests carried out at a temperature of
40
C and a pressure of 45 mmHg made it possible to
separate a distillate containing only 1% of the organic
content and 20% of the ammonium. Metal content in
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