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The Treatment of Pulp and Paper Mill e Fluent
The Treatment of Pulp and Paper Mill e Fluent
Review paper
Abstract
The manufacture of paper generates signi®cant quantities of wastewater; as high as 60 m3 /tonne of paper produced. The raw
wastewaters from paper and board mills can be potentially very polluting. Indeed, a recent survey within the UK industry has found
that their chemical oxygen demands can be as high as 11 000 mg/l. This paper reviews the processes involved in paper making and
examines the eects which they could have on the environment. It also evaluates the treatment processes which are used to minimise
these eects. In line with the majority of UK practice, it focuses mainly on aerobic biological treatment and, in particular, on the
activated sludge process. This means that there is an in-depth discussion about the problems associated with ®lamentous bacteria
and sludge ``bulking''. The paper also discusses the way in which anaerobic digestion can be applied to the treatment of liquid wastes
from the manufacture of paper. Ó 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Paper and board mills; Wastewater treatment; Activated sludge; Anaerobic digestion
0960-8524/01/$ - see front matter Ó 2001 Elsevier Science Ltd. All rights reserved.
PII: S 0 9 6 0 - 8 5 2 4 ( 0 0 ) 0 0 0 6 0 - 2
276 G. Thompson et al. / Bioresource Technology 77 (2001) 275±286
Table 2
Imports/exports and consumption of wood and wood products in the UK (millions of cubic metres) (data from Forestry Commission Facts and
Figures; www.forestry.gov.ukwww.forestry.gov.uk)
Year Import Exports UK production Apparent consumption
Wood Pulp Panels Paper Total Total
1991 16.0 8.7 4.9 13.6 43.2 5.0 6.5 44.8
1992 15.6 8.7 4.9 14.3 43.5 5.1 6.6 45.0
1993 15.0 7.8 4.8 14.6 42.2 4.5 6.8 44.5
1994 17.4 8.6 5.1 16.4 47.6 5.8 7.3 49.0
1995 14.1 9.1 5.41 15.9 44.3 6.0 7.6 45.8
1996 15.0 8.2 5.4 16.6 45.1 5.4 7.1 46.7
1997 15.6 8.4 6.0 17.8 47.7 6.8 7.4 48.3
G. Thompson et al. / Bioresource Technology 77 (2001) 275±286 277
Fig. 1. Speci®c water usage (mean values) (data from Anon., 1997).
Fig. 3. Pulp production in western Europe (data taken from European
Commission, 1996).
1.1.2. Papermaking
Western Europe plays an important role in the global
paper industry being the second largest producer and
consumer of paper, with North America being the
largest. Together they control a 60% share of the worldÕs
paper market. Western Europe produces some 80 106
tonnes of paper and board each year. This accounts for
Fig. 2. Speci®c euent production (mean values) (data from Anon.,
1997).
approximately a quarter of the worldÕs total paper
production. The Nordic countries contribute about 30%
of the annual European production. Japan is the third
most important producer with 12% of total production
Table 3 (European Commission, 1996) (Fig. 4).
Untreated euent loads from pulp and paper manufacture (range of
In the production of paper, pulp is diluted to at least
design values)a (data from Billings and DeHaas, 1971)
99% with water and a mineral ®ller; china clay, titanium
Paper type kg/tonne of product
dioxide or chalk; and water-soluble substances such as
Suspended solids 5-day BOD optical brighteners and polyvinyl alcohol are added
Pulps (Hentzschel et al., 1998). This is then pumped to a
Bleached groundwood 20±38 11±26 headbox and is distributed evenly along a moving wire
Textile ®ber 130±220 90±130
Straw 180±220 180±220
cloth. This even distribution is facilitated by the con-
De-inked 180±360 26±70 stant side-to-side movement and vibration aorded by
Fine papers 22±45 7±18 the headbox. The majority of the water drains through
Book/publication papers 22±45 9±22 the wire leading to the formation of a wet paper sheet.
Tissue paper 13±45 4±13 This is then vacuum dried and pressed, to extract more
Coarse papers
Boxboard 22±30 9±18
water and form the paper sheet. Residual water is re-
Corrugating brand 22±30 11±26 moved by passing it through a series of steam-heated
Newsprint 9±26 4±9 cylinders.
Insulating board 22±45 67±110 Recycled paper is an important source of cellulose
a
Design value is dependent upon yield. ®bre for certain paper and board grades (corrugated
278 G. Thompson et al. / Bioresource Technology 77 (2001) 275±286
Other problems, which may arise, occur when the that UK mills will be authorised under the EC directive
treatment processes employed to treat the pulp and on integrated pollution prevention and control (IPPC),
papermill euent fail. This can result in the release of with emission data being available for public scrutiny
suspended solids, and the loss of nutrients, such as ni- via a Europe-wide Polluting Emissions Register. The use
trogen and phosphorus, which can lead to eutrophica- of primary treatment followed by secondary biological
tion in recipient bodies. treatment, which is the approach adopted by UK mills,
The Environmental Protection Act, 1990, introduced is considered to be BATNEEC for the industry.
integrated pollution control (IPC) to the UK. The aim
of IPC was to prevent pollution at source and protect
the environment overall (air, water and land) from cer- 2. The treatment of pulp and papermill euent
tain prescibed processes and substances. Control of
pollution is, therefore, ``integrated'' to achieve the best The main treatment process used at pulp and paper-
environmental outcome. A number of UK mills were mills plants is primary clari®cation, and in some cases, it
authorised under IPC. As part of this authorisation is then succeeded by secondary treatment, generally of a
process, mills had to demonstrate that they were using biological nature (Fig. 5). Tertiary processes for further
best available techniques not entailing excessive cost treatment, or colour removal, are rare at present, but
(BATNEEC) to control emissions to the environment. may become more common in the future if legislation
As part of the process, data on environmental emissions becomes more stringent.
were made available by papermills to the Environment
Agency (EA) for public scrutiny via the Chemical Re- 2.1. Primary clari®cation
lease Inventory. The IPC is underpinned by a series of
guidance notes, relating to the classes of industrial Primary clari®cation may be achieved by either sed-
processes, which set out the EA view of what are con- imentation or ¯otation. Within the papermills surveyed
sidered to be BATNEEC for a particular process and in the UK, sedimentation was the preferred option.
which indicate resultant emission levels. It is also likely These units achieved a high removal of suspended solids,
Fig. 5. Generalised schematic diagram of the plant for the treatment of papermill euent.
280 G. Thompson et al. / Bioresource Technology 77 (2001) 275±286
Table 4
Activated sludge operating parameters
Mill type
Recycled ®bre, Printings/writings Printings/writings Tissue Other
Sludge age (d) 5±8 6±18 7±40 20±30
HRT (h) 8±12 5±30 11±18 50±200
Volumetric loading (kg/m3 d) 0.5±0.8 0.4±1.4 naa 1.2
Hydraulic loading (m3 /d) 28,800 0.04±1.25 naa 1220
Sludge loading/d 8.6 tonne 0.07±0.25 naa naa
DO concentration (mg/l) 0±6 0±7 0.5±9 0.1±9.9
COD (mg/l) 1500±1900 1060±2770 50±2000 0±11,000
Sulphate (mg/l) 500 140±1050 525±1750 6750
Ammoniacal-nitrogen (mg/l) 6 naa 1.90±2.70 16.5
Nitrate (mg/l) 2.50 naa 3±13.5 82.5
Phosphate (mg/l) 2.18 naa 9.9±20.3 12.3
MLSS (mg/l) 3000±7000 2300±9000 3000±6000 2200±5350
SSVI at 3.5 g/l 48±90 30±160 50±130 72±360
a
Data are unavailable.
G. Thompson et al. / Bioresource Technology 77 (2001) 275±286 281
Table 6
Operating parameters, wastewater characteristics and predominant types of ®lamentous microorganisms
Operating conditions or wastewater characteristics Predominant types of ®lamentous microorganisms
Low dissolved oxygen concentration in activated sludge S. natans, Type 1701, Type 1863 and possibly Type 021N, Thiothrix
Low organic loading of activated sludge M. parvicella, H. hydrossis, Types 0041, 0092, 0581, 0961, 0675, 0803, 1851
N or P de®ance in wastewaters S. natans, Type 021N and possibly Thiothrix
Increased concentration of sulphide in wastewaters Thiothrix, Beggiatioa, possibly Type 021N
282 G. Thompson et al. / Bioresource Technology 77 (2001) 275±286
5. Some ®laments exhibit a preference for low concen- many countries, as can be seen from its ranking in the
trations of DO. This is especially notable at the inlet three surveys on bulking and ®lamentous bacteria
zone of aerators. (Table 7).
6. Some ®laments have a competitive edge in a low nu- N. limicola II has not been evaluated to the same
trient environment and it has been suggested that to- extent as other ®lamentous species. Indeed, there ap-
tal inorganic nitrogen should be >1 mg/l and soluble pears to be only one report of its growth characteristics
orthophosphate phosphorous >0.2 mg/l. in pure culture (Nowack and Brown, 1990). However,
7. Temperature will aect the growth rates of the bacte- recent work has shown that in mixed liquor, its com-
ria so that dierent species will become dominant at petitive advantage can be controlled by increasing the F/
dierent times of the year. M ratio (Scruggs and Randall, 1998).
8. Nutrient gradients in the aeration tank will favour Sludge bulking can also be controlled by the instal-
non-®lamentous species. Therefore, con®gurations lation of a selector or by the addition of chemicals such
which create plug-¯ow characteristics in the aeration as chlorine, ferrous salts or lime. The use of selectors is
tank are preferable. one of the most widely accepted procedures for the
A survey of nine papermills in 1994 identi®ed poor control of bulking (Forster, 1996; Dalentoft and Thulin,
oxygenation, low organic loading rates and nutrient 1997a; Marten and Daigger, 1997; Prendl and Kroiss,
de®ciencies as the main causes of bulking (Cingolani 1998; Shao and Jenkins, 1989). The selectors are placed
et al., 1994) and a study of pulp and papermill activated prior to the aeration tank and can be aerobic, anoxic or
sludge plants around the Great Lakes showed that anaerobic. The primary aim of a selector is to supress
stress, resulting from low phosphorus concentrations, the growth of ®laments in favour of ¯oc-forming bac-
produced bulking caused by N. limicola III (Richard and teria. The higher growth rate for ¯oc-formers is utilised
Cummins, 1997). under conditions with a high substrate concentration.
Type 021N is often classi®ed as a nutrient de®ciency These conditions are created by imposing a high in-
bulking ®lament. It has been found to be very common stantaneous food to mass ratio on the biomass. Marten
in conventional treatment plants (Table 7) and can and Daigger (1997) have shown that the target F/M for
usually be controlled by means of a selector (see later: an anoxic selector is 0.7±1.2 kg BOD/kg MLSS d and
Neilson et al., 1998). The reduction of sulphate by the that this, coupled with an aerobic solids retention time
sulphate-reducing bacteria is also linked to the domi- of 8±12 days, will successfully control bulking ®laments.
nant growth of 021N. Yamamoto et al. (1991, 1994, The use of chemicals, as a short-term solution to control
1996) have shown that: the eects of bulking, will improve settleability without
1. as sulphate reduction increased, the growth of 021N the destruction of the ®lamentous bacteria. Simpson
in activated sludge increased and the sludge settle- et al. (1991) have reported that the SVI of sludges from
ment deteriorated (1991); two trial works where bulking was occurring could be
2. sulphate reduction is the trigger for ®lamentous bul- reduced by treatment with an iron-rich mixture of metal
king by 021N (1994); salts.
3. there is a symbiotic relationship between the sul- Another option is to kill the ®lamentous bacteria
phate-reducing bacteria and the ®lamentous sulphur selectively by the addition of toxic substances such as
bacteria (1996). chlorine and hydrogen peroxide. The use of chlorine is
Types of industrial waste which promote Type 021N widely practiced, especially in the US, and can generally
bulking typically contain soluble, readily biodegradable, be dosed in the returned activated sludge stream enter-
carbonaceous substrates and a high sulphate concen- ing the aeration tank (Neethling et al., 1985; Jenkins
tration. Bulking from Type 021N often has a rapid et al., 1986). The main chemical used in the UK is so-
onset, 2±4 days, is severe, sludge volume index dium hypochlorite. The use of hydrogen peroxide is not
(SVI) > 500, and is persistent (Richard et al., 1985). as common.
H. hydrossis is related to a low food to microorgan- An alternative method is to use some form of solids±
ism ratio. It has been found to be the cause of bulking in liquid separation process other than gravity sedimenta-
tion. In recent years, research has concentrated on the
Table 7 use of ultra®ltration (Ragona and Hall, 1998). The ul-
Relative signi®cance of ®lamentous bacteria in bulking situations tra®ltration membrane acts as a barrier for microor-
Species Survey ranking ganisms: thus, any pollution in the ®nal euent will be a
Germany Netherlands USA (Jenkins result of soluble components only. If this method were
(Wagner, (Eikelboom, et al., 1986) to be employed, the growth of ®lamentous bacteria
1982) 1982) would cease to be of any concern.
021N 1 6 3 Changing the operational con®guration of the acti-
H. hydrossis 6 2 9 vated sludge plant can also in¯uence the settlement
N. limicola 7 11 12
characteristics of the sludge. Sequencing batch reactors
G. Thompson et al. / Bioresource Technology 77 (2001) 275±286 283
are a time-orientated rather than a space-orientated followed by a conventional activated sludge system. The
version of the activated sludge process (Dennis and Ir- load applied to the Kaldnes-tank was 10±15 kg COD/m3
vine, 1979) and in laboratory studies, they have been d and that to the activated sludge system was 0.1±0.4 kg
shown to be more resilient to shock loads of KME than COD/m3 d (Dalentoft and Thulin, 1997b). The use of
aerated lagoons (Weeks and Oleszkiewicz, 1993). Ar- the Kaldnes process as a pre-treatment can also aect
guably, the ®ll mode is the most important phase of the the characteristics of the subsequent activated sludge.
process. It can be done with no aeration, with partial Dalentoft and Thulin (1997b) have shown that, in such a
aeration or with full aeration. Of these, the unaerated ®ll process stream, when the Kaldnes stage was out of op-
mode has been shown to prevent ®lamentous bulking eration, the SVI of the sludge in the activated sludge
(Norcross, 1992, Yu and Gu, 1996). This technology aeration tank was >300. When both the processes were
does not appear to be used by the UK paper industry, in operation, the SVI was around 120.
but it is a process which is used in Canada (Cocci et al., Other types of bio®lm process have also been used in
1998) and it has been reported that its use has reduced the treatment of papermill wastewaters. For example,
capital costs by about 30%, compared to conventional high-performance trickling ®lters using plastic media
secondary treatment systems (Villeneuve and Tremblay, have been used successfully as a pre-treatment stage
1995). The best sludge settlement properties and highest prior to an activated sludge plant (Moebius et al., 1990).
COD removal were found to occur with a sludge age of Biological aerated ®lters (BAF) have also been used to
20 days, a ®ll-phase of 30 min and a react-phase of 12 h treat wastewaters from papermills. As is shown in Fig. 8,
(Franta and Wilderer, 1997). mean removal eciencies of >80% for both COD and
The Kaldnes process can be thought of as another BOD could be achieved with hydraulic retention times
activated sludge variant and is one which has success- (HRT) of about 0.75 h. (Kantardjie and Jones, 1997).
fully been applied to the treatment of papermill wastes
(Dalentoft and Thulin, 1997b). In eect, the process is 2.2.2. Anaerobic treatment
converted from one which is ¯oc-based to one based on Anaerobic digestion is a process frequently employed
attached bio®lms. This is done by introducing a plastic for the secondary treatment of industrial wastewaters
support medium (approximately 10 mm diam: 7 mm), but, whilst investment in this technology is increasing
either into the aeration tank itself or into a separate tank (Pearson, 1990), it is not used as widely as the activated
which preceeds the main aeration tank. Typically, the sludge process by the pulp and paper industry. It has
media occupies 67% of the tank volume and will provide many potential advantages in comparison to aerobic
a speci®c surface area of about 500 m2 /m3 . The eect of treatment, such as lower sludge production, lower
doing this is to increase the mass of biological solids chemical consumption, smaller land requirements due to
available for degrading the pollutants in the wastewater. smaller reactors and energy production in the form of
This, therefore, means that higher loads can be applied. methane. Typical COD removal data for the treatment
The results from one full-scale plant at a mill producing of papermill wastewaters shows that a relatively con-
customised ®ne paper show a COD removal eciency of stant removal eciency of about 80% can be achieved
85±95%. The plant was con®gured as a Kaldnes-tank and that the treated euent has a COD concentration of
about 800 mg/l (Fig. 9). This COD concentration means Treatment Directive for COD are applied. Even after
that some form of additional treatment is required. In full biological treatment, the euent from a papermill
Netherlands, Industriewater Eerbeeck operate an an- can contain appreciable concentrations of COD. For
aerobic up¯ow sludge blanket reactor as a pre-treatment example, a study by Oeller et al. (1997) has reported
for the euents from three papermills before the ®nal data from six papermills showing COD:BOD ratios
treatment in a ®ne bubble diused air activated sludge ranging from 67:1 to 14.5:1. Treated papermill euents
plant (Paasschens et al., 1991). can contain colour. This may come from the production
The high sulphur content of pulp and paper mill ef- of coloured toilet tissue or from lignin (Franta et al.,
¯uent might seem to suggest that anaerobic treatment 1994). In the UK, regulatory bodies are moving towards
would not be an appropriate treatment option because stringent colour standards based on River Quality Ob-
of the potential for hydrogen sulphide production jectives. These are based on speci®ed absorbances at a
(Lettinga et al., 1991). However, the work reported by range of wavelengths (Churchley, 1994). In the future,
Hamm et al. (1991) suggested that H2 S toxicity was less toxicity-based consents may also be imposed (Wharfe
important than the eect of high concentrations of Ca and Tinsley, 1995).
and SOÿÿ 4 . Sulphide removal has also been achieved in The main tertiary treatments which have been em-
reactors based on the colourless sulphur bacteria which ployed to date at a few sites in the industry are mem-
convert the sulphide ions to elemental sulphur (Buisman brane processes, especially ultra®ltration. This process is
et al., 1991). Using bio®lm reactors, removal eciencies a pressure driven separation, based on the selective
of up to 90% were obtained with hydraulic retention permeability of a membrane, which can serve as a sec-
times as low as 19 min. Chen and Horan (1998a) have ondary clari®er as the ®nal liquid±solids separation step.
reported the use of a two-stage anaerobic±aerobic ap- Numerous physico-chemical processes have also been
proach to remove COD and sulphate from the waste- developed to remove a variety of toxic materials from
waters generated at an integrated newsprint mill. COD pulp euents and to reduce parameters such as colour
and sulphur removals were 66% and 73%, respectively. and COD. They include ozonation and adsorption, of-
In general, anaerobic digestion is carried out at meso- ten in combination with coagulation, which is used as a
philic temperatures, 35±37°C. However, the use of the pre-treatment stage. A study by Chen and Horan
thermophilic temperature range is worth considering (1998b) compared the use of ozone and coagulation and
(Rintala et al., 1991) as it will give faster reaction rates demonstrated that chemical coagulation followed by
and a higher gas production rate. dissolved air ¯otation and multimedia ®ltration would
be the most suitable tertiary treatment option. Dissolved
2.2.3. Alternative processes air ¯otation, coupled with coagulation with alum and an
Although activated sludge plants have been the most organic polymer, were also selected as the tertiary
common wastewater treatment process, there are several treatment option for the Braviken papermill in Sweden
problems with the process. It produces sludges with very and gave ®nal COD concentrations of <100 mg/l
variable settlement properties, it is sensitive to shock (Thoren et al., 1997). Research by Hostachy et al. (1997)
loading and toxicity, and its capacity to remove poorly has shown that ozonation is particularly eective
biodegradable toxic substances is limited. Studies were whereas Oeller et al. (1997) showed that COD removal
conducted in Finland on the use of pre-ozonation to eciencies achieved by ozone were variable.
prevent process failure, to improve the puri®cation ef-
®ciency and to reduce pollution to receiving water-
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