International Research Journal of Applied and Basic Sciences © 2016 Available online at www.irjabs.com ISSN 2251-838X / Vol, 10 (1): 32-43 Science Explorer Publications

Assessment of physico-chemical characteristics and treatment method of Paper Industry Effluents :

a review

Azimvand J*1, Mirshokraie SA2

1*. Corresponding author , Ph.D student, Dept. of chemistery, Payame Noor University, Tehran, Iran. 2. Professor, Dept. of Chemistry, Payame Noor University, Tehran, Iran.

Corresponding Author email: ch.azimvand@yahoo.com

ABSTRACT: The wastewaters generated from production processes of this industry include high concentration of chemicals such as sodium hydroxide, sodium carbonate, sodium sulfide, bisulfites, elemental chlorine or chlorine dioxide, calcium oxide, hydrochloric acid, colour, very high level of Biochemical Oxygen Demand (BOD), Chemical Oxygen Demand (COD) ,due to presence of lignin and its derivatives from the raw cellulosic materials , chlorinated compounds, suspended solids (mainly fibres), fatty acids, tannins, resin acids, sulphur and sulphur compounds, etc. The major problems of the wastewaters are high organic content (20-110 kg COD/air dried ton paper), dark brown coloration, adsorbable organic halide (AOX), toxic pollutants, etc . Biological treatment has for some time been state of the art for effluent treatment but as energy costs are soaring new ways of minimizing treatment costs are sought. Increased water reuse by closing up water circuits without ruining the quality of final products is an important aspect. Pretreatment of selected process streams prior to external treatment will in many cases be beneficial from both cost and environmental points of view. Both aerobic and anaerobic treatment systems are feasible to treat wastewater from all types of pulp and paper mills except that bleaching kraft effluents are less suitable for treatment by anaerobic means, as they are more toxic to anaerobic bacteria. The anaerobic treatment of high strength wastewater requires further treatment as it contains high residual COD. A combination using an anaerobic process followed by an aerobic treatment system is a better option, as it can make use of the advantages of both the treatment processes. Color is removed efficiently by fungal treatment, coagulation, chemical oxidation, and ozonation. Chlorinated phenolic compounds and AOX can be removed by adsorption, ozonation and membrane filtration. Combinations of two or more physicochemical processes produce a high removal of toxic pollutants. Combinations of physicochemical and biological treatment processes with optimization of the process provide a long-term solution for pulp and paper mill effluent treatment. Keywords: paper industry, Physico-chemical parameters, Wastewater, physical,biological and Physicochemical treatments

INTRODUCTION

Pulp and paper industry is considered as one of the most polluter industry in the world (Thompson et

al., 2001; Sumathi & Hung, 2006). The production process consists two main steps: pulping and bleaching. Pulping is the initial stage and the source of the most pollutant of this industry. In this process, wood chips as raw material are treated to remove lignin and improve fibers for papermaking. Bleaching is the last step of the process, which aims to whiten and brighten the pulp. Whole processes of this industry are very energy and water intensive in terms of the fresh water utilization (Pokhrel & Viraraghavan, 2004). Water consumption changes depending on the production process and it can get as high as 60 m

3/ton paper produced in spite of

the most modern and best available technologies (Thompson et al., 2001). The environmental problems of pulp and paper industry are not limited by the high water consumption.

Wastewater generation, solid wastes including sludge generating from wastewater treatment plants and air emissions are other problems and effective disposal and treatment approaches are essential. The significant solid wastes such as lime mud, lime slaker grits, green liquor dregs, boiler and furnace ash, scrubber sludges, wood processing residuals and wastewater treatment sludges are generated from different mills. Disposal of these solid wastes cause environmental problems because of high organic content, partitioning of chlorinated organics, pathogens, ash and trace amount of heavy metal content (Monte et al., 2009).

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Many kinds of the wastes as summarized above are generated from different processes. The amount, type and characteristics of these wastes are important to provide the best treatment technology. Physicochemical and biological treatment technologies are used extensively for the pulp and paper mills. The lab-scale and full-scale studies about sedimentation/floatation, coagulation and precipitation, adsorption, chemical oxidation and membrane filtration were carried out in the literature to examine physico-chemical approach (Pokhrel & Viraraghavan, 2004). Biological treatment both aerobic and anaerobic technologies are preferred for treatment of pulp and paper mills because of wastewater composition consisting of high organic compounds and economical aspects. Additionally, some fungi species are used to remove color and AOX from the effluents (Taseli and Gokcay, 1999). In some countries, tertiary treatment is applied to obtain discharge limits of regulations (Thompson et al., 2001). Finally, the wide application in the full-scale plants for treatment pulp and paper mills is hybrid systems, which is combined physico-chemical and biological treatment alternatives (Pokhrel & Viraraghavan, 2004).

Disposal strategy of solid wastes generated from pulp and paper industry is varied depends on the country and the regulations obeyed. After sorting and handling, dewatering, thermal application such as combustion and anaerobic digestion to obtain energy and deposit in landfills are general applications. However, the solid wastes should be monitored after landfill deposition because of toxic characteristics of the compounds (Monte et al., 2009). Waste characterization and source

Pollution from the pulp and paper industry can be minimized by various internal process changes and management measures such as the Best Available Technology (BAT). Dube et al. (2000) reported a 60% reduction in effluent BOD due to an internal process change in Irving Pulp and Paper Limited,Canada. The estimated data by Springer (2000) showed that the water use in the US in 1959 was about 250 m3/adt whereas water use in 1995 was reduced to 50 m3/adt. However, the average water use for the pulp and paper mills in India was still 200 –259 m3/ton of paper production (Welander, 2000). Several authors have suggested internal process change as a measure to control pollution (Reilama and Ilomaki, 1999; Webb, 1994; Dey et al., 1991). Raghuveer and Sastry (1990) reported BOD, COD, and color reduction by internal management measures. However, the treatment of the wastewater by various external processes is essential. Since pulp and paper industry discharges varieties of pollutants, the treatment methods also vary.

Pulp and paper industry is one of the most water and energy consuming industry in the world. This industry uses the fifth largest energy consumer processes; approximately 4% of total energy is used worldwide. Also during pulp and paper process, the important amount of waste is produced. It has been estimated that 500 million tons of paper and etc. per year will be produced in 2020. Three different raw materials are used in the pulp and paper industry as nonwood fibers and wood materials; soft and hard woods. Waste and wastewaters are generated from both of pulp and bleaching processes. Additionally, 100 million kg of toxic pollutants are released every year from this industry (Cheremisinoff & Rosenfeld, 1998). Manufacturing technologies and process description

Pulping process is the first step of the production. The main steps of this part are debarking, wood chipping, chip washing, chip digestion, pulp screening, thickening, and washing. Mechanical and chemical operation processes in pulping are used in the worldwide. While mechanical processes involve mechanical pressure, disc refiners, heating, and light chemical processes to increase pulping yield; wood chips are cooked in pulping liquors at high temperature and under pressure in the chemical pulping processes. (Sumathi & Hung, 2006). Additionally, mechanical and chemical processes can be combined in some applications. The yield of mechanical processes is higher (90-95%) compared to chemical processes (40-50%). However quality of the pulp obtained from mechanical processes is lower and also the pulp is highly coloured and includes short fibers (Pokhrel & Viraraghavan, 2004). Therefore, chemical pulping carrying out in alkaline or acidic media is mostly preferred. In alkaline media generally referred as Kraft Process, the woodchips are cooked in liquor including sodium hydroxide (NaOH) and sodium sulfide (NaS2). Mixture of sulphurous acid (H2SO3) and bisulfide ions (HSO3

-) is used in acidic media named as sulfide process. During the pulp processing, approximately 5-10% of the lignin comes from the raw materials cannot be

removed and these are responsible from the dark colour of the end product. The production of white paper (pulp bleaching) includes five or optional six treatment steps with sequentially elemental chlorine, alkali, optional hypochlorite stage, chlorine dioxide, alkali and chlorine dioxide .

Wood is the most abundant source of papermaking fiber. Wood consists of various compounds (lignin, carbohydrate, and extractives) which are hard to biodegrade, and these derivatives are washed away from the fibers during the washing, dewatering, and screening processes. Depending upon the type of the pulping process, various toxic chemicals such as resin acids, unsaturated fatty acids,diterpene alcohols, juvaniones, chlorinated resin acids, and others are generated in the pulp and paper making process. The pollutants at various stages of the pulping and paper are presented in Fig. 1.

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It is clear that an individual pulping stage generates different quantities, qualities and types of pollutants. The wastewater pollution load from individual pulping and papermaking process is given in Table 1.

Figure 1. Pollutants from various sources of pulping and papermaking (US EPA, 1995).

Table 1. Typical wastewater generation and pollution load from pulp and paper industry (Rintala and Puhakka, 1994)

COD (kg/adt pulp)

SS (kg/adt pulp)

Wastewater (m3/adt pulp or paper)

Process

5 – 20 nr 5 – 25 Wet debarking 15 – 32 nr 10 – 15 Groundwood pulping 40 – 60 10 – 40 10 – 30 TMP -unbleached 50 – 120 10 – 40 10 – 30 TMP-bleached 70 – 120 20 – 50 10 – 15 CTMP-unbleached 100 – 180 20 – 50 10 – 15 CTMP-bleached 30 – 120 3 – 10 20 – 80 NSSC nr 20 – 50 80 – 100 Ca-sulfite (unbleached) 120 – 180 20 – 60 150 – 180 Ca-sulfite (bleached) 60 – 120 10 – 40 40 – 60 Mg-sulfite (unbleached) 40 – 60 10 – 20 40 – 60 Kraft-unbleached 100 – 140 10 – 40 60 – 90 Kraft-bleached nr nr 10 – 50 Paper making

1000 – 1100 50 – 100 200 – 250 Agrobased small paper mill

nr—not reported; adt—air dry ton; NSSC—neutral sulfite semi-chemicals.

Wastewater characteristics

Different pulping processes utilize different amount of water and all of these processes are water intensive. The quality of wastewater generated from pulping and bleaching is significantly distinctive because of the process and chemical types (Billings and Dehaas, 1971).

Approximately 200 m3 water are used for per ton of produced pulp and most of them are highly

polluted, especially wastewater generated from chemical pulping process (Cecen et al., 1992). Wood preparation, pulping, pulp washing, screening, washing, bleaching, paper machine and coating operations are

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the most important pollution sources among various process stages. Wastewaters generated from pulping stage include mostly wood debris, soluble wood materials, and also some chemicals from chemical pulping process. Bleaching process wastewater has a different quality. These wastewaters are not higher strength than pulping process wastewater, however they include toxic components.

The wastewaters generated from pulping process consist various wooden compounds such as lignin, carbohydrate and extractives and the treatment of these wastewaters by biologically is difficult. Addition of them, some toxic compounds such as resin acids, unsaturated fatty acids, diterpene alcohols, juvaniones, chlorinated resin acids, and others can exist in the wastewaters subjecting to the process (Pokhrel & Viraraghavan, 2004). The most important reaction in the bleaching step is oxidation of chlorine and the main problem about the wastewater content is chlorinated organic compounds or AOX (Sumathi & Hung, 2006).

The toxic effects of these by-products in the wastewaters on environment have been studied. Various studies reported that fish living in pulp and paper industry wastewaters have toxic/lethal effects on the daphnia, fish, planktons and other bioata in the receiving water bodies (Owens et al., 1994; Hickey and Martin, 1995; Yen et al., 1996; Vass et al., 1996; Liss et al., 1997; Lindstrom-Seppa et al., 1998; Leppanen and Oikari, 1999; Johnsen et al., 1998; Erisction and Larsson, 2000; Schnell et al., 2000b; Kovacs et al., 2002).

The characteristics of the wastewater generated from various processes of the pulp and paper industry depend upon the type of process, type of the wood materials, process technology applied, management practices, internal recirculation of the effluent for recovery, and the amount of water to be used in the particular process. As an example, Mohamed et al. (1989) reported that the load of chlorinated phenols and acids in the wastewaters of hardwood kraft mill was three to eight times lower than it was in the soft wood kraft mill. The general characteristics of the wastewater produced at various process stages and pollution sources are given in Tables 2, 3 and 4.

Table 2. Typical characteristics of wastewater (mg/l) at different processes (Bajpai, 2000)

Table 3. Characteristics of wastewater (mg/l) at various pulp and paper processes

Table 4. Characteristics of wastewater at various pulp and paper processes

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Solid and hazardous wastes Wastewater and consequently solid wastes are the main environmental problem of the pulp and paper

mills because this industry has a very water intensive production processes (Cabral et al., 1998; Thompson et al., 2001). Solid wastes from pulp and paper industries are mainly treatment sludges, lime mud, lime slaker grits, green liquor dregs, boiler and furnace ash, scrubber sludges, and wood processing residuals. Wastewater treatment sludges have a significant concern for the environment because of including chlorinated compounds (EPA, 2002). The characteristics of all solid waste generated from the pulp and paper mills are organic exception of boiler and furnace ash. The chemicals of the solid wastes are varied depends on the process type. Solid wastes, sources and qualities are given in Table 5.

Table 5. Solid waste types and sources from pulp and paper mills (EPA, 2002; Nurmesniemi et al., 2007) Source Waste Type Waste characteristic

Wastewater treatment plant

sludge

Organic fraction consistes wood fibers and biosludge Inorganic fraction consists clay , calcium carbonate and other materials 20-60% solid content PH=7

Caustic process Dregs , muds Green liquor dregs consisting of non reactive metals and insoluble materials lime mud

Power boiler ash Inorganic compounds

Paper mill sludge Colour waste and fibre clay including slowly biodegradable organics such as cellulose , wood fibres and lignin

Treatment strategies

Although the best approach is to minimize the waste generation from the pulp and paper mills and to recycle, the treatment applications are still necessary. In this section, up-to date treatment technologies are given. Wastewater treatment

End of the pipe pollution treatment strategies are necessary to provide the discharge limits. The general flow-chart of a typical wastewater treatment plant is given Figure 2.

The main treatment application for wastewater generated from pulp and paper process is primary and secondary treatment. However, tertiary treatment can be an obligation in future due to possible new legislations. The physicochemical step is rare at present.

Figure 2. Flow scheme of general wastewater treatment plant of pulp and paper industry (End of the pipe (EOP) pollution

treatment) (Cabral et al., 1998; Thompson et al., 2001)

Primary Treatment (physical)

In this step, the aim is to remove suspended solid such as bark particles, fiber, fiber debris, filler and coating materials and consequently organic materials. Primary clarification can also be achieved without sedimentation and flotation. However Thompson et al. (2001) mentioned that sedimentation is generally

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preferred application for the pulp and paper mills in UK and approximately 80% of suspended solid was removed successfully. Also Rajvaidya and Markandey (1998) reported 70-80% of removal in the sedimentation. Dissolved air flotation and filtration are the other option as primary treatment for pulp and paper mills. Secondary Treatment (biological)

Aerobic lagoons, activated sludge systems, anaerobic treatment and sequential biological treatment (aerobic-anaerobic or anaerobic-aerobic) are the most common biological treatment application for pulp and paper mills. In this section, the details of these processes are given and they are discussed(Pokhrel,T.Viraraghavan,2004 ). Activated Sludge Systems

This conventional treatment system is used in treatment of several industrial wastewater types in order to remove COD, BOD, SS, and AOX. There are a lot of studies in the literature to show the treatability of pulp and paper mills by activated sludge system. Some of them focused on the BOD, COD, AOX and other specific compound removal under different operation conditions. Schnell et al. (1997) showed that 74% of filtered COD, nearly %100 BOD5, resin and fatty acid removal were achieved in the full-scale plant. Saunamaki (1997) reported that 82% and 60% COD removal efficiency at paper mills and pulp mills, respectively in full-scale activated sludge systems of Finland. Knudsen et al. (1994) claimed high COD and BOD removal efficiency by two stage activated sludge process. Also Hansen et al. (1999) and Chandra (2001) showed similar results. The other part of these studies focused on the removal of AOX and other specific compounds such as chlorinated phenols, guaiacols, catechols, vanillins, 1,1-dichlorodimethyl sulfone (DSS), and chlorinated acetic acid (Mohamed et al., 1989; Demirbas et al., 1999; Bajpai, 2001; Chandra, 2001). The main operational problems of the pulp and paper mills are macro nutrient (N and P) limitation in the systems and growth of the filamentous microorganisms and bulking problems. The nutrient limitation problem is overcome by addition of nutrient. However, the dosage is important point on this step because the external addition causes adverse environmental effects such as eutrophication. Cingolani et al. (1994) highlighted that the main causes of bulking in the pulp and paper mills treatment are poor oxygenation, low organic loading rates and also nutrient limitations. This problem can also be controlled by installation of a selector or addition of chemicals such as chlorine, ferrous salts, lime or talk powder. Selectors are mostly preferred application for bulking (Forster, 1996; Marten and Daigger, 1997; Prendle and Kroiss, 1998; Andreasen et al., 1999). Aerated Lagoons (Stabilization Basins)

Aerated lagoons are the simple and economical biological systems and they have been studies very well as lab-scale and full-scale at the pulp and paper mills. These systems have been used for removal of BOD, low-molecular weight AOX and fatty acids at full-scale applications (Bajpai, 2001). Stuthridge and Macfarlane (1994) showed that 70% of AOX could be removed efficiently in a short residence time. Welander et al. (1997) reported that COD removal was achieved as 30-40% in a full-scale lagoon and 60-70% in a pilot-scale plant. Lab-scale treatability studies were conducted by Chernysh et al. (1992) to monitor the AOX and TOC removal of bleached kraft effluent. Slade et al. (1999) also reported three aerated stabilization basins, which treated elemental chlorine free (ECF) integrated bleached Kraft mill effluents. Anaerobic Treatment Processes

Anaerobic treatment processes are more suitable for treatment of high strength wastewater such as pulp and paper mills. In the literature, there are a variety of studies on the anaerobic treatability and microbial community of this type of effluents (Poggi-Varaldo et al., 1996; Bajpai, 2000; Ince et al., 2007). Also, anaerobic microorganisms are more efficient than aerobics in order to degrade chlorinated organic compounds. However, the sulphur content in the wastewaters is the main disadvantages for application of anaerobic systems, because one of the end products is hydrogen sulphide in the anaerobic biodegradation in the presence of sulphate (Lettinga et al., 1991). Although Hamm et al. (1991) reported that the toxic effect of H2S is less than high concentration of Ca

2+ and SO4

2-. The other important issues for the application of anaerobic treatment in

pulp and paper mills are toxicity of wastewater, anaerobic biodegradability characteristic of specific waste types such as lignin derivates, resin and fatty acids, loading capacity, response to loading fluctuation, and recovery of energy and chemicals (Sumathi and Hung, 2006). Several hundred tons of inorganic chemicals per day for delignification are used in a conventional pulp and paper mill. So, the recovery and reuse of these chemicals are one of the most economical and environmental concern. Addition of it, the black liquor is rich in lignin and a conventional pulp and paper mill produces 1.7-1.8 tons dry solid of black liquor per ton produced pulp and the potential energy of this liquor from anaerobic digestion is 250-500 MW (Stigsson, 1998; Larson et al., 2000). Anaerobic contact reactor, up-flow anaerobic sludge blanket (UASB) reactor, anaerobic filter, and fluidized bed reactor are mostly employed reactor types in pulp and paper mills.

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Fungal Treatment Fungal species have been used to remove colour and COD from pulp and paper mills (Eaton et al.,

1980; Livernoche et al., 1983; Wang et al., 1992; Gokcay and Dilek, 1994; Duran et al., 1994; Sakurai et al., 2001). Pencillium sp., P. chrysosporium and white rod fungi are the most widely used species. Choudhury et al. (1998) reported that Pleurotus ostreatus was removed 77% of lignin, 76.8% of BOD, 60% of COD, and 80% of colour. Tertiary Treatment (Physicochemical)

Physicochemical treatment processes include removal of suspended solids, colloidal particles, floating matters, colors, and toxic compounds by either sedimentation, flotation, screening, adsorption, coagulation, oxidation, ozonation, electrolysis, reverse osmosis, ultra-filtration, and nano-filtration technologies(Pokhrel, T. Viraraghavan,2004) . Coagulation/Precipitation

Coagulation and flocculation is normally employed in the tertiary treatment in the case of pulp and paper mill wastewater treatment and not commonly adopted in the primary treatment. Tong et al. (1999) and Ganjidoust et al. (1997) carried out a comparative study of horseradish peroxide (chitosan) and other coagulants such as (Al2(SO4)3), hexamethylene diamine epichlorohydrin polycondensate (HE), polyethyleneimine (PEI), to remove adsorbable organic halides (AOX), total organic carbon (TOC), and color. The authors indicated that modified chitosan was far more effective in removing these pollutants than other coagulants. Wagner and Nicell (2001) investigated the treatment of foul condensate, defined by phenolic compounds, and toxicity using microtox assay from kraft pulping by horseradish peroxide and H2O2 and found a total phenol reduction below 1 mg/l and toxicity (microtox assay) reduction by 46%. Dilek and Gokcay (1994) reported 96% removal of COD from the paper machine, 50% from the pulping, and 20% for bleaching effluents by using alum as a coagulant. Rohella et al. (2001) stated polyelectrolytes were better than the conventional coagulant alum to remove turbidity, COD, and color. Sheela and Distidar (1989) reported on black liquor treatment by precipitation with CaSO4Á2H2O in the presence of CO2. The removal of dissolved solids was reported to be 63%. However, Wang and Pan (1999) reported that the use of coagulants such as polyethylene oxide (PEO), worsened the settlability and increased COD levels, turbidity, and suspended solids of the treated effluent when the dose was between 25 and 250 ppm. Chernoberezhskii et al. (1994) reported that coagulation with aluminum sulfate or modified adsorbents was the best option for color removal from the sulfate and sulfite wood pulp and paper industry. Adsorption

Murthy et al. (1991) reported a high removal of color by activated charcoal, fuller’s earth, and coal ash. Shawwa et al. (2001) reported 90% removal of color, COD, DOC, and AOX from bleached wastewater by the adsorption process, using activated coke as an adsorbent. Sullivan (1986) concluded that the waste- water produced by the Union Camp Facility at Franklin, VA, can be treated by activated carbon and ion exchange to reduce color and chloride to levels acceptable for reuse. Das and Patnaik (2000) investigated the lignin removal efficiency of the blast furnace dust (BFD) and slag by the adsorption mechanism. Their study showed 80.4% and 61% removal of lignin by BFD and slag, respectively. Narbaitz et al. (1997) reported that PACTk process was an effective process to remove AOX from the kraft mill effluent to meet Ontario’s year 2000 regulation (AOX: 0.8 kg Cl/adt of production). Chemical Oxidation

Balcioglu and Ferhan (1999) reported on photo-catalytic oxidation of kraft pulp bleaching wastewater showing that the removal largely depended on the concentration of COD and chloride below a certain level. Zamora et al. (1998) reported on the use of horseradish peroxide to decolorize kraft effluent by 50% within three hours of reaction time. The degradation of phenolic and polyphenolic compounds present in the bleaching effluent was studied using advanced oxidation systems such as photocatalysis with O2/ZnO/UV, O2/TiO2/UV, O3 and O3/UV. The authors concluded that O2/ZnO/UV and O2/TiO2/UV were the best systems to oxidize the effluent in a short period of time. Perez et al. (2002c) reported that the combination of Fenton and photo-fenton reactions proved to be highly effective for the treatment of bleaching kraft mill effluent. Verenich et al. (2000) reported on the improvement in biodegradability of an effluent from 30% to 70% by wet oxidation method. Hassan and Hawkyard (2002) studied the removal of color by combined oxidation with ozone and Fenton’s reagent and stated that 100% color removal wasachieved at a pH of 4 – 5 in the case of ferral (derived from natural clay sources, which contains 2% ferric sulfate and 6% aluminum sulfate) and ferric sulfate. Dufresne et al. (2000) reported on the oxidation of total reduced sulfur (TRS) giving odor free products by catalytically enhanced oxidation.

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Membrane Filtration Membrane filtration is a potential method to remove colour, COD, AOX, salts, heavy metals, and total

dissolved solids from pulp and paper mills (Zaidi et al., 1992; Afonso and Pinho, 1991; Falth, 2000; Merrill et al., 2001). The effluent of membrane filtration can be used again in production process or discharge directly to the receiving water bodies. Dube et al. (2000) showed that 88% and 89% removal of BOD and COD, respectively was achieved by reverse osmosis (RO). Ozonation

Yeber et al. (1999) reported that a substantial removal of COD, TOC, and toxicity from pulp mill effluent and increased biodegradability of the effluent were achieved after treatment with ozone. Korhonen et al. (2000) reported a 90% removal of ethylenediaminetetraacetic acid (EDTA) and a 65% removal of COD by ozone treatment of the pulp mill effluent. Hinck et al. (1997) reported that neither EDTA nor diethylene triamine pentaacetic acid (DTPA) are biodegraded in aerobic conditions. Oeller et al. (1997) reported high removal of COD and DOC from the pulp effluent by ozone treatment. Freire et al. (2000) reported a 12% reduction of total organic carbon, total phenols reduced to 70%, and effluent colors to 35% of bleached pulp mill effluent after 60 min of ozonation. Several authors reported on toxic compounds, COD, and color removal by ozone treatment (Hostachy et al., 1997; Zhou and Smith, 1997; Yamamoto, 2001). Roy-Arcand and Archibald (1996) reported that biotreated kraft effluents yielded a substantial decrease in the biologically recalcitrant residual adsorbable organic halogens (AOX), converted COD to BOD and yielded large decrease in color. Verenich S, Laari A (2000) investigated the removal of lipophilic wood extractives from TMP wastewater by ozonation. The authors indicated that a high dosage of ozone (100 –300 mg/dm3) was required to remove 50% of lippphilic wood extractives. Korhonen and Tuhkanen (2000) reported that ozone doses of 0.2 mgO3/initial mgCOD eliminated over 90% resin acid. Perez M, Torrades et al. (2001a) reported high removals of TOC, COD, AOX, and color from bleached kraft mill effluent (BKME1) using heterogeneous photocatalysis and ozone treatment. Sevimli and Sarikaya (2002) reported a 95–97% color removal for high doses of ozone in 15 min of ozonation. Kallas and Munter (1994) suggested post treatment of bleached mill effluent by ozonation and adsorption. Management and disposal of solid wastes

Integrated solid waste management of pulp and paper mills are through anaerobic digestion, composting, land applications, thermal processes such as incineration/combustion, pyrolysis, steam reforming, and wet oxidation.

Anaerobic Digestion: This process type is a cost effective way due to the high-energy recovery (Verstraete and Vandevivere, 1999; Mata-Alvarez et al., 2000). Industrial wastes, which have high organic content and digestable, are suitable for anaerobic digestion like paper sludge and wastewater treatment plant sludge (Kay, 2003; CANMET, 2005).

Composting: This method is suitable for the wastes and sludge, especially paper fibres and organic materials. The wastes are stabilized via microorganisms with minimal carbon loss. The end product of this process, humus-like material, can be used for houseplants, greenhouse and agriculture (Jokela et al., 1997; Hackett et al., 1999; Christmas, 2002; Gea et al., 2005).

Land Application: This method has been preferred disposal method, especially for the acidic soil due to CaCO3 content of sludge. This application is widely used in the United Kingdom and Northern Europe. Before the application, dewatering and/or incineration treatment are done to the waste/sludge in order to reduce volume (Carr and Gay, 1997; Van Horn, 1997).

Incineration (Combustion): Combination of incineration with power and steam generation is one of the most applied methods in Europe, especially for wastewater treatment plant sludge. However, water and ash content of most sludges cause the energy deficiency. Fluidized bed boiler technology is becoming the one of the best solution for the final disposal of paper mill wastes in order to provide successful thermal oxidation of high ash, high moisture wastes (Busbin, 1995; Fitzpatrick and Seiler, 1995; Davis et al., 1995; Porteous, 2005; Oral et al., 2005).

Pyrolysis: In this process, organic wastes are converted to gaseous and liquid phase under high temperature and in the absence of oxygen. This is an alternative technology to incineration and landfill. This method is suitable for organic content high wastes such as wood, petroleum, plastic waste. However this technology is not sufficient for pulp and paper mill waste. Some investigations have been continue to adapt this technology to pulp and paper mills (Frederik et al., 1996; Fytili and Zabaniotou, 2008).

Steam Reforming: This technology is used for sludge treatment, however it is still considered as an emerging technology for paper sludges. Steam reforming is a novel combustion technology, which carries out in a steam reforming reaction system (Durai-Swamy et al., 1991; Demirbas, 2007).

Wet Oxidation: The principle of wet oxidation is that organic compound as solid or liquid form is firstly transferred to water where it contacts with an oxidant under high temperature and pressure. During wet oxidation, waste pulped with water is carbonized and its fuel value increases to the equivalent of medium-grade

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coal. The waste does not cause any air emission in order to combust without flame or smoke (Pokhrel, T. Viraraghavan,2004). This technology is also considered as an emerging technology like steam reforming.

CONCLUSION

The paper demand increases every day as a result of developed population and industrialisation. Water and energy utilization and in particularly waste generation are becoming more important concern ever worldwide. A major goal is to decrease damage to environment by waste minimization, reuse and recycle. To use best available techniques and innovative methods is becoming more an issue. However, end-of-pipe Biological treatment is still the major approach to minimize the risk. To evaluate pollutants and to develop treatment technologies need a holistic approach.

The major pollution load constitutes wastewaters from pulp and paper mills. A variety of wastewater is generated from diverse processes. Different technologies and their combinations have been used for their treatment. The most common applied systems are biological treatment, sequential anaerobic and aerobic systems, followed after primary treatment. Solid waste management and disposal are also another concern. During the final disposal step, the aim should be chemical compound and energy recovery because of environmental and economical aspects. However, the waste minimization has still the first and important approach.

The best available treatment technology for all three waste phases depends on the production processes, raw materials and the regulations, which the industries have to obey.

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