Desalination 246 (2009) 7886

Demonstration of a treatment system for purification and reuse of laundry wastewater

I. Ciabattia,*,1, F. Cesarob, L. Farallia, E. Fatarellaa, F. Tognottia
a

Next Technology Tecnotessile Societ Nazionale di Ricerca r.l., via del Gelso 13, 59100 Prato, Italy Tel. +39-0574-634040; Fax +39-0574-634045; email: chemtech@tecnotex.it b Studio Tecnoacque, Via Roma 78, 35040 Boara Pisani (Padova), Italy
Received 17 June 2008; revised 06 February 2009; accepted 09 February 2009

Abstract A pre-industrial scale experimentation aimed at the demonstration of a system for purification and reuse of wastewater from an industrial laundry was carried out by means of a prototype plant installed in situ, fed with 15 m3/h of untreated wastewater. The tested treatment system consisted of: (i) physico-chemical pre-treatment (coagulation, flocculation and Dissolved Air Flotation or DAF); (ii) sand filtration; (iii) ozonation; (iv) Granular Activated Carbon (GAC) filtration and (v) cross-flow ultrafiltration (UF) on flat membranes realised in polyvinyledene fluoride (PVDF). Under the optimised treatment conditions, it was demonstrated that the outlet of the GAC filter meets the requiring law limits for discharge to surface waters in Italy, even in terms of residual content of total surfactants (<2 mg/L). The post-treatment of ultrafiltration on flat membranes further reduced the residual pollutant content, allowing reuse of the treated effluents in some washing processes of home textiles, as demonstrated by whiteness index measurements. A cost analysis was performed to assess the operating costs of each treatment step. Keywords: Industrial laundry effluent; Ozonation; Activated carbon filtration; Membrane filtration; Purification; Reuse

1. Introduction Water has always played a major role in industrial laundry operations, due to the large quantity of this universal solvent required for the effective
*Corresponding author.
1

laundering of industrial garments and other textile goods. On the average, a laundry uses 15 L of water to process 1 kg of work and discharges a total of 400 m3 of wastewater daily. Treatment of this kind of wastewater is particularly difficult because of the high surfactant content, together

Present address: European Commission, Research Executive Agency, rue de la Loi 200, 1049 Brussels, Belgium. Tel. +32-2-2994247; email: ingrid.ciabatti@ec.europa.eu Presented at the conference Engineering with Membranes 2008; Membrane Processes: Development, Monitoring and Modelling From the Nano to the Macro Scale (EWM 2008), May 2528, 2008, Vale do Lobo, Algarve, Portugal.
0011-9164/0X/$ See front matter 200X Elsevier B.V. All rights reserved. doi: 10.1016/j.desal.0000.00.000

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with the high organic and inorganic load generated by the soil that has been washed out. It has been reported that wastewater from a laundry, where very dirty items are being washed, contains mineral oils, heavy metals and dangerous substances that have chemical oxygen demand (COD) values of 120020,000 mg/L, whilst laundries that wash items from households and hotels generate effluents with COD values of 4001200 mg/L [1]. Different methods of pre-treatment are used to purify industrial laundry wastewater before it is discharged. The complexity of pre-treatment varies from location to location depending on the size of the facility, the volume of water and chemicals consumed, the type and usage of products used by the customers being serviced, and the specifics of national and local law requirements. One of the most widely used pre-treatments of industrial laundry wastewater consists of coagulation and flocculation, followed by Dissolved Air Flotation (DAF). Coagulation is a wellknown treatment which, by addition of a chemical (such as Al3+ and Fe3+ salts or organic polymers), destabilises small particles in suspension. Such particles after electrical neutralisation tend to gather and form coagulated flocs of 2050 m in size. Flocculation reagents, consisting of long-chain polymers or polyelectrolytes, reinforce the floc formation and cohesion [2]. Flotation allows then to separate the flocs from the liquid; as solid/liquid separation system, flotation is preferred to settling being the coagulums very light [3]. The coagulationflocculationflotation system may be insufficient for treating the highly variable industrial laundering effluents in agreement with the legislation for wastewater discharge in force in the European Union (EU) Member States. In particular, with this kind of treatment process, industrial launderers might periodically exceed the values of parameters such as suspended solids and Biochemical

Oxygen Demand (BOD) and therefore incur in the related municipal sewer surcharges. This fact, together with increasing costs associated with water supply in the EU, is dictating the need for European industrial launderers to address water conservation and recycling as matters of increasing priority. In this framework, the present paper refers to a pre-industrial scale validation of a treatment system for reuse of industrial laundry effluents realised within the European project PROWATER, that has been co-financed by the European Commission within the LIFE Environment Programme. The investigated treatment system was composed of: (i) physico-chemical pre-treatment (coagulation, flocculation and DAF); (ii) sand filtration; (iii) ozonation; (iv) Granular Activated Carbon (GAC) filtration and (v) ultrafiltration (UF) on flat membranes. Ozonation is considered one of the most promising oxidation processes with which to control the levels of organic pollutants in water. It can also be used for the removal of inorganic species, as an aid to the coagulationflocculation processes [4]. It has been found that the reaction between ozone and water pollutants occurs either by direct oxidation (pH < 6) or by an indirect pathway (pH > 6), whereby hydroxyl radicals resulting from the decomposition of ozone serve as oxidants through chain reactions [5]. Because of its strong oxidative properties, ozone has been investigated for treatment of several types of wastewater, e.g. effluents containing phenols [6,7], pesticides [8,9] and dyes [10,11]. Activated carbon, also called activated charcoal or activated coal, is a general term which covers carbon material derived from sources such as almonds, coconuts, walnut hulls, other woods and coal. It is a particularly good adsorbent medium thanks to its high surface area-tovolume ratio: 1 g of a typical commercial activated carbon will have a surface area equivalent to 1000 m2. Adsorption on GAC has been

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found to be an effective technology for treating water contaminated with taste and odour-causing compounds, organic chemicals, chlorinated compounds and even metals [1214]. The superiority of activated carbons in the removal of surfactants from laundry effluents compared to other adsorbents has been reported in literature [15]. The proper selection of cost-effective GAC and the operational parameters of the filtration are critical to the successful operation of large-scale GAC adsorbers. Ultrafiltration is a pressure-driven membrane technique that is used for the separation from a liquid of material in the 1 nm to 10 m size range (Molecular Weight Cut Off, or MWCO, of about 2000500,000). It is widely used in drinking water [16,17] and wastewater [18,19] treatment. In the field of textile effluent purification, it has been mainly proposed as pre-treatment to nanofiltration (NF) or reverse osmosis (RO) for wastewater reuse [20,21]. The UF+RO combination has also been investigated on lab scale for reuse of laundry effluents [1]. A combination of the technologies presented in this paper (with the exception of GAC filtration) was successfully validated on pre-industrial scale for the treatment and reuse of real dyeing [22] and finishing [23] effluents. The objective of the experimentation described here has been to adapt and optimise such approach to wastewater originated by laundry operations, leading to the demonstration of a treatment system applicable to several kinds of industrial effluents.
Table 1 Characteristics of the kind of stream investigated

2. Materials and methods 2.1. Wastewater characteristics The industrial laundry participating in this study LIT S.r.l. (Turin, Italy) is specialised in wet washing of textiles made of vegetable fibres, animal fibres, man-made fibres and their mixtures. Each day LIT washes some 22 tons of textiles, using both conventional washerextractors and continuous-batch washers. The production cycle requires a total of 400 m3/day of water. At present, the water needs of the company are covered by wells. Before being fed to the laundry machinery, well water is softened by ion exchange resins and then collected in a storage tank. In addition to surfactants, the washing cycle foresees the use of other chemicals such as softeners, oxidants/disinfectants (sodium hypochlorite and hydrogen peroxide), alkali, acetic acid, oxalic acid, formic acid, which are found as pollutants in the resulting wastewater. Table 1 reports the typical range of some parameters of the endof-pipe laundry effluents considered in the study. 2.2. Products As primary coagulant, both aluminium polychloride and a commercial mixture of it were tested. In both cases, different dosages were investigated by preliminary jar tests to select the best product and the best conditions, which were then verified by pre-industrial scale tests. As secondary coagulant, a polyamine-based product was used. Again, different dosages were

pH 79
a

COD (mg/L) 4001000

Total suspended solids (mg/L) 90200

Turbidity (NTU)a 40150

Conductivity (S/cm) 13003000

Absorbance at 420 nm 0.010.05

Non-ionic surfactants (BIAS) (mg/L) 110

Anionic surfactants (MBAS) (mg/L) 115

Nephelometric turbidity unit.

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investigated by jar tests and the best conditions were validated by pre-industrial scale trials. Considering both the technical and economic issues, the best solution was found to be the addition of 750 parts per million (ppm) of aluminium polychloride as primary coagulant and the addition of 90 ppm of polyamine-based product as secondary coagulant. An anionic polyelectrolyte was dosed on-line as flocculant (addition: 3 ppm) in the prototype. Ozone was produced from a generator fed with liquid oxygen (maximum ozone production: 550 g/h); additions ranging from 30 to 90 ppm were tested. The addition of 40 ppm of ozone was found to be the most suitable one, considering both the technical and economic aspects. Alkaline solutions added with sodium hypochlorite were used for chemical cleaning of the UF membranes. 2.3. Large-scale prototype A large-scale prototype (maximum water feed: 15 m3/h) was installed at LIT in order to validate on-site the proposed system for treatment and reuse of laundry effluents. Upstream the prototype, a metallic grid (0.75 mm) was used to remove the coarse materials. The prototype consisted of the following sections: (1) coagulation, flocculation and dissolved air flotation; (3) sand filtration; (4) ozonation and (5) GAC filtration. Ozone was introduced into the wastewater stream by ceramic dishes. Part of the effluent of the GAC filter (0.7 m3/h) was fed to a UF Flamec module by Filterpar (Italy), featuring commercial cross-flow flat membranes (total filtration area: 48 m2). The membranes of this system are made of polyvinyledene fluoride (PVDF) and have a Molecular Weight Cut-Off (MWCO) of 20 kDa. Permeation is realised by an extraction pump working under vacuum. The liquid to be filtered is partly re-circulated by a low head pump. The hydraulic performance of the UF section of the prototype was monitored over time.

2.4. UF membrane cleaning An optimised chemical cleaning procedure was applied for the maintenance of the filtration performance of the UF membranes. In particular, the chemical cleaning was realised when a reduction of 20% of the normalised permeate flux was observed. The adopted cleaning protocol realised with chemicals from Everblue S.r.l. is described below: 1. Alkali cleaning for biofilm removal with 20 L solution of 1%v/v of EB-Cleaner B1 and 1%v/v of EB-Cleaner B2 at pH = 11 and at T = 40C. A 20% of the solution is fluxed through the membranes and re-circulated for at least 2 h. 2. Non-oxidant biocide for fungi and bacterium removal with a 20 L solution of 0.02%v/v of EB-Biocide 10 at T = 40C. A 20% of the solution is fluxed through the membranes and re-circulated for at least 0.5 h. 3. Iron and organic deposit removal with 20 L solution of 1%v/v of EB-Cleaner B1 and 1%v/v of EB-Cleaner B2 at pH = 11 and at T = 40C. A 20% of the solution is fluxed through the membranes and re-circulated for at least 2 h. 4. Acid cleaning for iron and inorganic deposit removal with a 20 L solution of 2%v/v of EB-Cleaner A1 at T = 40 C. A 20% of the solution is fluxed trough the membranes and re-circulated for at least 2 h. 2.5. Effluent analyses The following parameters of interest were determined on untreated effluents and after the different purification steps of the system: pH; temperature; COD, according to test method DIN 38409; turbidity, as per IRSA 2120; Total Suspended Solids (TSS), according to IRSA 2050; conductivity; absorbance at 420 nm; anionic surfactants, as Methylene Blue Active Substances

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45 40 35 30 25 20 15 10 5 0 0

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Permeability [L/(m2h bar)]

20

40

60

80 [m3]

100

120

Permeate production

Fig. 1. Trend of the UF membrane permeability when filtering laundry effluents at LIT.

(MBAS) determined as per ISO 7875-1; nonionic surfactants by the Bismuth Active Substance (BIAS) method. In some cases, other parameters of interest were measured, e.g. ammonia nitrogen, according to test method DIN 38406 and total phosphorous, according to test method DIN 38408. 2.6. Reuse tests One hundred per cent UF permeate was used in washing experiments of home textiles realised with a washerextractor processing 100 kg of textiles. The final rinsing was realised using softened well water. The experiments with the UF permeate were compared to the same kind of processes realised with primary water. The white index of the

washed textiles was determined as per [24], to provide a quantitative assessment of the tests. 3. Results and discussion 3.1. Ultrafiltration performance The UF membranes featured a pure water permeability of 84 L/(hm2bar). Figure 1 shows the trend of the membrane permeability when filtering the laundry effluents pre-treated by flotation, ozonation and GAC filtration (mean parameters of the membrane feed are presented in Table 2 as GAC filter outlet). As shown in the figure, after filtration of about 20 m3 of wastewater, the permeability to the laundry effluents decreased of about 25% compared to the initial value of the

Table 2 Mean values of some parameters of interest for the prototype influent, the outlet of the GAC filter and the UF permeate Limits for discharge to Values for surface water reuse 5.59.5 <160 <80 <15 <10 <2 6.58.5 <100 <5 <2 <2000 <20

Parameter pH COD (mg/L O2) TSS (mg/L) Turbidity (NTU) Conductivity (S/cm) Ammonia nitrogen (mg/L NH4+) Total phosphorous (mg/L P) Total surfactants (mg/L)

Influent 7.2 602 166 110 1342 1.8 1.9 8.78

Outlet GAC filter 7.4 140 4 1.1 1275 0.13 0.45 1.60

UF permeate 7.3 81 2.5 0.8 1127 1.00

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100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0%

83

Removal efficiency

COD

Outlet flotation tank Outlet ozonation tank

Outlet GAC filter

UF permeate

Fig. 2. COD removal efficiency from laundry wastewater after the different purification steps realised in series by the prototype at LIT.

test, as the membranes had became fouled. Membrane fouling could be explained by the adsorption of residual surfactants onto the membranes, due to both hydrophobic and electrostatic interactions in case of ionic surfactants. On this regard, it is to be noticed that anionic surfactants are widely used in washing operations, as they are particularly effective at oily soil cleaning and clay soil suspension, and therefore they are found in higher concentration in the resulting effluent compared to the nonionic surfactants (Table 1). To limit membrane clogging, periodic regenerations of the membranes with washing solutions featuring alkali were realised after permeation cycles of about 100 m3 of water.

3.2. Pollutant removal efficiency Water quality parameters were controlled by means of sampling of both the prototype influent (equalised end-of-pipe wastewater) and the outlets of the different sections of the prototype, connected in series, in order to monitor their contribution to the overall performance of the treatment system. For the main parameters of interest, Figs. 2 4 report the removal efficiency , that was calculated according to the equation: (%) = (C0 CF)/C0 100, where C0 is the initial

concentration of the pollutant and CF is the final value. To be noted that C0 is always referred to the prototype influent (untreated wastewater after pH regulation by H2SO4 and homogenisation), whilst CF relates to the effluent of the considered treatment section. A mean COD removal efficiency of 87% was obtained with the overall system (Fig. 2). The physico-chemical pre-treatment alone has a COD removal efficiency of 45%. Thanks to the following sand filtration, ozonation and GAC filtration, total COD removal efficiency reached 77%, meeting the Italian legal limit for discharge to surface waters (160 mg/L). Finally, UF allowed to further decrease the residual COD, reaching an average value < 100 mg/L, as wished by the involved industrial laundry to realise a partial wastewater reuse. The purification system also reached a high removal efficiency of TSS (98%) and turbidity (99%), as shown in Fig. 3. The physico-chemical pre-treatment played a major role in removing these parameters (removal efficiency of 88% and 94% for TSS and turbidity, respectively). This was possible thanks to the selection of proper coagulants and to the use of relatively high doses, needed to limit the ozone consumption (and related cost) in the downstream ozonation step. Thanks to the following treatments of sand filtration, ozonation and GAC filtration, TSS and turbidity were almost completely

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TSS 100% 90% Removal efficiency 80% 70% 60% 50% 40% 30% 20% 10% 0% Outlet flotation tank

Turbidity

Outlet ozonation tank

Outlet GAC filter

UF permeate

Fig. 3. Removal efficiency of total suspended solids and turbidity from laundry wastewater after the different purification steps realised in series by the prototype at LIT.

removed, hence UF had almost no effect on these parameters. Decrease in total surfactants was also significant: mean removal efficiency of 87% and 93% for non-ionic and anionic surfactants, respectively, were obtained (Fig. 4). For these parameters, an important contribution came from ozonation and GAC filtration, allowing to meet the Italian legal limit for discharge to surface water (total surfactants < 2 mg/L). A further reduction occurred by UF (surfactants decreased of the half compared to UF feed), possibly explaining the fouling by their adsorption onto the membrane.
BIAS 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% Outlet flotation tank Outlet ozonation tank Removal efficiency

Colour and microbiological analyses confirmed the good performance of the proposed system. Table 2 reports the mean values of some parameters of interest which relate to: (A) prototype influent; (B) outlet of the GAC filter; (C) UF permeate; versus both the Italian legal limits for discharge to surface waters and the target values for partial reuse in washing processes defined by the laundry participating in the study. As shown by the table, the outlet of the GAC filter met the Italian legal limits for discharge to surface water, whilst the target values for reuse were reached thanks to the final UF treatment.
MBAS

Outlet GAC filter

UF permeate

Fig. 4. Removal efficiency of non-ionic surfactants (as BIAS) and anionic surfactants (as MBAS) from laundry wastewater after the different purification steps realised in series by the prototype at LIT.

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3.3. Reuse tests Washing tests of home textiles including bed linen and wipes were carried out with the UF permeate to verify the possibility to realise a partial wastewater reuse. The final rinsing was realised with primary water. According to both the visual check of the washed items by the technicians of the laundry and the measurements of the white index (in case of bed linen, equal to 100.946 when using primary water and to 102.528 when using the UF permeate), it has been demonstrated that the proposed treatment system allows to produce an effluent suitable for reuse. 3.4. Cost assessment A cost assessment of the proposed system was carried out. It resulted that the maximum operating costs for the different treatment sections are: (i) physico-chemical pre-treatment: 0.42 Euro/m3; (ii) sand filtration: 0.04 Euro/m3; (iii) ozonation: 0.10 Euro/m3; (iv) GAC filtration: 0.09 Euro/m3; (v) UF: 0.16 Euro/m3. Hence, the total operating costs of the proposed approach amount to 0.81 Euro/m3. 4. Conclusions Under tested conditions, a purification system composed of: physico-chemical pre-treatment; sand filtration; ozonation and GAC filtration; allows to meet the requiring law limits for discharge to surface waters in Italy. A post-treatment of ultrafiltration on flat PVDF membranes allows reuse of the treated effluents in some washing processes; however, the need for a frequent membrane chemical washing has to be taken into account when considering a full scale implementation. Acknowledgements The authors wish to thank the LIFE Environment Programme of the European Commission

for co-financing the PROWATER project, which has received an award as Best of the Best LIFE Environment Project 20072008. Edoardo Cornaglia and Bruno Villa (LIT S.r.l.) and all other project partners are gratefully acknowledged for their support.

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