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Process integration in bleaching section of paper mill for minimization of

fresh water consumption and wastewater generation

Article  in  Environmental Engineering and Management Journal · December 2013

DOI: 10.30638/eemj.2013.295

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Environmental Engineering and Management Journal December 2013, Vol.12, No. 12, 2435-2442
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“Gheorghe Asachi” Technical University of Iasi, Romania

PROCESS INTEGRATION IN THE BLEACHING SECTION OF A PAPER

MILL FOR MINIMIZATION OF FRESH WATER CONSUMPTION
AND WASTEWATER GENERATION

Sudheer Kumar Shukla1,2, Deepak Kumar3, Vivek Kumar3,

Mukesh Pandey4, Mukesh Chandra Bansal3
1
Sungkyunkwan University, School of Mechanical Engineering, Republic of Korea
2
Yonsei University, Department of Civil and Environmental Engineering, Seoul, 120-749, Republic of Korea
3
Indian Institute of Technology Roorkee, Department of Paper Technology, Saharanpur Campus, Saharanpur-247001, India
4
Rajiv Gandhi Technical University, School of Energy and Environment Management, Bhopal, India

Abstract

Water system integration can minimize both fresh water consumption and wastewater discharge from the paper mills. In the
present study, Pinch Technology was used to analyze and optimize the water network of an integrated paper mill. A system was
developed and a limiting constraint (COD concentration) was identified based on investigations for water quality, and then
minimum fresh water and wastewater targets were determined without considering water losses. The analysis was extended by
estimating the additional input of fresh water required to balance the actual water losses. A nearest neighbor algorithm (NNA)
was used to distribute the fresh and recycled water in the plant operations. Results showed that the flow rates of fresh water could
be decreased up to 20.83 %.

Key words: mass load, process integration, pinch analysis, water conservation, water network

Received: March, 2010; Revised final: August, 2012; Accepted: August, 2012

1. Introduction regulatory agencies. Environmental and economic

considerations have made the reuse of process water
The pulp and paper industry is one of the 17 necessary in the operation of pulp and paper mills. In
most polluting industries according to the Central recent years, there have been considerable
Pollution Control Board (CPCB) of India. Huge developments in systematic approaches to minimize
quantity of water is used in the manufacture of pulp the use of fresh water and the production of
and paper. Used water leaves as wastewater, unless it wastewater by the pulp and paper industry. There is
is appropriately recycled. The paper mill effluent also a growing public concern over the quality of the
carry high pollution load in terms of COD (chemical environment (Gavrilescu et al., 2012; Goldblatt et al.,
oxygen demand), BOD (biochemical oxygen 1993; Hallale, 2002). The process integration
demand), and AOX (adsorbable organic halides). The approach is often used to implement water recycling.
effluent is dark brown in color mainly due to the In this approach, recycled water is used in operations
lignin and lignin derivatives (Kulkarni, 2003). that produce high levels of contaminants (Gavrilescu
The pulp and paper industry is facing a major et al., 2008; Wenzel et al., 2002). Two main types of
problem because of the increasing scarcity of water methods are used for the systematic design of water-
and stringent discharge standards introduced by recovery networks: (i) rigorous graphical targeting


Author to whom all correspondence should be addressed: E-mail: [email protected]; [email protected];
Phone: +82-31-299-4194
 Shukla et al./Environmental Engineering and Management Journal 12 (2013), 12, 2435-2442

approaches (Aly et al., 2005; El-Halwagi, 1997; Successful applications of water network
Prakash and Shenoy, 2005; Wang and Smith, 1994) synthesis in various process industries have been
and (ii) mathematical-based optimization techniques documented for both the water pinch and
(Keckler and Allen, 1999). A systematic approach to mathematical optimization approaches, including
develop optimal water recycling in an industrial plant petrochemical complexes (Liu et al., 2005; Mann and
comprises of two main tasks (Dunn and Wenzel, Liu, 1999), chemical manufacturing (Feng et al.,
2001). The first task is to define the maximum 2006; Forstmeier et al., 2005; Ku-Pineda and Tan,
amount of recycling that is possible and the second 2006; Mann, 2003), oil refineries (El-Halwagi et al.,
task is to design alternative recycling network that 1992; Wang and Smith, 1994), a steel plant (Tian et
will allow the operations to meet the water-recycling al., 2008), and pulp and paper mills (Chiang et al.,
target. Wang and Smith (1995) studied operations 2006; Delgado et al., 2006; Foo et al., 2006; Jacob et
with a fixed flow rate and suggested the use of local al., 2002; Lovelady et al., 2007; Manan et al., 2007;
recycling and the splitting of water-using operations Manan et al., 2007; Parthasarathy and
to meet flow rate constraints. El-Halwagi et al. Krishnagopalan, 2001; Yang et al., 2000).
(2003) presented a rigorous graphical targeting For applications of different approaches in the
approach that minimized the use of fresh resources paper industry, Koppol et al. (2003) applied a
by means of segregation, mixing, and direct recycling mathematical programming approach in a non-bleach
and reuse strategies. Dhole et al. (1996) also paperboard mill and Parthasarathy and
proposed targeting methodology for networks, Krishnagopalan (2001) applied an approach
involving operations with a fixed flow rate. Polley consisting of a graphical solution strategy followed
and Polley (2000) improved the work carried out by by mathematical optimization using a non-process
Dhole et al. (1996) and demonstrated that to element (chloride) as key contaminant for the paper
minimize consumption of fresh water, it is necessary mill using the kraft pulping process. Shafiei et al.
for the outlet streams to leave at their maximum (2004) applied a genetic algorithm coupled with
allowable concentration. Alva- Argáez et al. (1998) linear programming in an integrated newsprint paper
presented a solution for multi-component systems mill based on thermo-mechanical pulping and
based on mathematical programming. In addition, considered TDS as the contaminant. Foo (2007)
Alva-Argáez et al. (1999) used simplifying demonstrated the application of the WCA technique
assumptions to propose a trans- shipment model. using Parthasarathy and Krishnagopalan (2001) as a
Savelski and Bagajewicz (2000a, b) showed that case study. Foo (2009) reviewed pinch analysis
outlet concentrations must equal their maximum techniques for water network designing extensively.
allowable values in an optimal water network. They Jeźowski (2010) discussed about network designing
identified the processes which need to be fed fresh methods for water recycling in his review. Tan et al.
water first and those processes which must receive (2007) used the WCA in the mill that produced paper
wastewater by introducing the concept of from old newspapers and magazines. TSS was
monotonicity in the process-to-process connections. selected as the main contaminant and a concentration
In addition, Gómez et al. (2001) provided an block diagram (CBD) method for network design
algorithmic procedure to address this matter. was used.
Bagajewicz and Savelski (2001) proposed a linear In the present study, the process integration
programming formulation of the problem based on approach was used to define a water conservation
the necessary conditions of optimality. target for an integrated paper mill. The study was
Prakash and Shenoy (2005) developed the carried out for a bleaching section of an integrated
nearest-neighbor principle to design minimum fresh paper mill. An optimal water network was designed
water networks for fixed contaminant load problems using the nearest neighbor analysis principle to
and fixed flow rate problems. Manan et al. (2004) minimize the consumption of fresh water and effluent
estimated the minimum water target using the Water generation.
Cascade Analysis (WCA) technique, which is a
numerical alternative to the graphical water targeting 2. Water network of the paper mill
technique and can quickly yield an accurate
estimation of the minimum water target, the pinch- Integrated pulp and paper mills, producing
point locations, and the water allocation target for writing and printing grade paper, have three major
maximum water recovery. Jacob et al. (2002) process sections: (i) pulp making (pulping), (ii)
analyzed the water network of pulp and paper bleaching, and (iii) paper making. In the pulping
processes using linear programming. A non-iterative section, wastewater, known as black liquor, is
algorithmic procedure was used to design water generated from pulping and pulp washing operations
utilization networks in refineries and process plants and sent to the recovery section. During recovery
(Savelski and Bagajewicz, 2001). Yang et al. (2000) operations, practically all the inorganic chemical is
proposed a mathematical optimization approach to recovered and water and organic matter is
design a wastewater reuse network for a cleaning and transformed into heat and steam. The paper-making
rinsing operation of an electroplating process, a section always uses excess water. However, excess
papermaking process, and a semiconductor water from the paper-making section, known as
manufacturing process.

2436
 Process integration in the bleaching section of a paper mill for minimization of fresh water consumption and wastewater generation

whitewater, is recycled at various points in the paper AOX and TDS were also analyzed for present
mill through short and long circulation loops. study and found that COD is a limiting factor for
The bleaching section of a paper mill present study. Moreover detrimental substances
generates highly colored effluent that cannot be sent (anionic oligomers and poly electrolytes as well as
to the recovery section. The bleaching operation in a nonionic hydro colloids) are known as anionic trash
typical paper mill first includes a delignification and are measured as cationic demand by
stage comprising of chlorination and alkali extraction polyelectrolyte titration in a streaming current device
followed by a second decolorizing stage. The mill or as chemical oxygen demand (COD).Water flow
selected for this study uses a conventional CEH rates and concentrations of COD in each inlet and
bleaching sequence. C, E, and H denote chlorination, outlet point of the bleaching section were measured
extraction and hypo-chlorination respectively. CE is (Table 1). COD is measured using a closed reflux
the delignification stage while H is the decolorizing method (APHA/AWWA, 1989).
stage. During the CEH bleaching sequence, pulp is As shown in Table 1, the problem is
subjected to chlorination first. Chlorinated pulp is characterized by a huge loss of water flow. The
washed and then subjected to extraction. Extracted problem can be characterized as a fixed flow rate
pulp is washed and then subjected to hypochlorite water network synthesis problem. Although some
treatment and finally washed for use in further predicted target impurity values, such as suspended
operations. The process flow diagram of CEH solids for paper machine showers, are available in the
bleaching is shown in Fig. 1. literature, however operational data were used in the
The major fresh water consumption points in present work to identify water-limiting data. Input
the bleaching section are the chlorine washer, alkali and output COD values were used as the sink and
washer, and hypochlorite washer. Pulp flows in C, E source concentrations, respectively.
and H reaction towers at different consistencies. Transformation of the water-limiting data into
Wastewater generated during different stages is a fixed load is shown in Table 2. Inlet and outlet
characterized by chemical characteristics such as pH, concentrations of COD (Table 1) were used as the
COD, AOX, TDS (total dissolved solids) and color, limiting concentrations and represented by Climi, in and
which can be identified as targeted impurities. For Climi,out , respectively. All three processes that
the present study, only COD was selected as the encounter water loss were segregated into two
single target impurity. Selection of process parameter individual processes, i.e., one with constant flow and
depends on streams involved in study. one with water loss (shown as a negative flow rate).

Fig. 1. Process flow diagram of CEH bleaching

Table 1. Process data for CEH bleaching

Mass Flow rate COD

Operation Inlet & Outlet
(t/d) (ppm)
Chlorine washer Inlet 4910 983
Outlet 3702 1190
Alkali washer Inlet 1930 1120
Outlet 747 2976
Hypo washer Inlet 1788 1078
Outlet 648 2176

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 Shukla et al./Environmental Engineering and Management Journal 12 (2013), 12, 2435-2442

Table 2. Essential process data for the water network design

Outlet flow rate Clim i,in x 103 (COD) Clim i,out x 103 (COD)
Process/Operation ∆m (kg/d)
(t/d) (ppm) (ppm)
Chlorination washer 1a 766 3702 983 1190
1b -1208 983 ----
Alkali washer 2a 1386 747 1120 2976
2b -1183 1120 ----
Hypo washer 3a 711 648 1078 2176
3b -1140 1078 ----

3. Calculation of minimum fresh water concentrations above the pinch point. The flow rate
consumption/wastewater production of water loss was calculated based on the principle of
conservation of mass (Mann and Liu, 1999), that is,
In the present study, targeting was carried out the mass load produced by the additional flow rate is
for the network using the mass problem table, which equal to that produced by the lost water.
is an algebraic targeting tool to locate the minimum Additional fresh water (Eq. 3):
fresh water flow rate for a fixed load problem (Castro
et al., 1999). The technique is easy to implement and lim
f  f loss  ( C pinch  Ckin ) /( C pinch  C0* ) (3)
readily extendable into a fixed flow rate problem
(Agrawal and Shenoy 2006; Liu et al., 2007) if the
water supply line is adjusted for water loss were f (t/d) = additional flow rate required to replace
experienced during the processes. The target for the loss, floss (t/d) is the actual loss of water in the
minimum fresh water is calculated without operation, and Cpinch = 2176 ppm is the concentration
considering water loss. Adjustment of the water at the pinch point, C*0 = conc. of COD in fresh water
supply for water loss was carried out using the is 30 ppm, and Climk, in = concentration in the kth
technique developed by Mann and Liu, (1999). interval from Table 2.
Essential data for the process integration study and Therefore, additional flow rates of water for
the water pinch analysis are presented in Tables 3 the chlorination, alkali, and hypo washers were
and 4, respectively. First, the limiting flow rate Fk calculated as: chlorine = f Chlorine loss [Cpinch–C limk,
*
(t/d) is determined by Eq. (1): in]÷[Cpinch–C 0]= 671.54 t/d; Alkali = 582.13 t/d; Hypo =
583.28 t/d.
Hence, the minimum mass flow rate of fresh
Fk  [ 1000 m k ,tot ]  ( C *k  C 0* ) (1) water = 671.54 + 582.13 + 583.28 + 1056.22 =
2893.17 t/d.
where C*0 = conc. of COD of fresh water = 30 ppm
and C*k = conc. of COD in kth interval in ppm. In 4. Water network synthesis
addition, ∆mk,tot = total mass load (kg/d) in the kth
concentration interval which equals ∆m1 + ∆m2 +∆m3 Prakash and Shenoy (2005) proposed a new
+ ∆m4 + - - - - - +∆mk and is determined by Eq. (2): algorithm, the nearest neighbor algorithm (NNA), for
optimizing the water network to meet the minimum
m k  f k
lim,
 ( C kout lim
 C kin )  1000 (2) fresh water target. The principle of the NNA states
that a particular water demand is satisfied by the
source stream which is nearest in terms of
where f k = total flow rate (t/d) of the operation contaminant concentration. In a problem with n
th
for the k concentration interval, and the values of sources and m demands, sources are serially
Climk,out and Climk,in are given in Table 2. The results numbered from S1 to Sn in order of increasing
of these calculations appear in Table 3. The arrows contaminant concentration and demands are similarly
represent the range of observed COD concentrations numbered from D1 to Dm. Fresh water is a source
within a process as given in Table 1. and is accordingly numbered S0.
The three operations were arranged in To fulfill the demand Dp in accordance with
ascending order of COD concentration. The the principle of nearest neighbors, two sources Sk and
maximum value of Fk = 1056.22 t/d was the apparent S(k +1) are chosen where Sk has a contaminant
minimum amount of fresh water required with no concentration just lower than the concentration of Dp
water loss from the system. The apparent minimum and S(k+1) has a contaminant concentration just
fresh and wastewater both equaled 1056.22 t/d, so the higher than that of Dp.
apparent pinch point occurred at the last The outlet flow of these operations required to
concentration interval, at a concentration of 2176 fulfill the inlet (in such a manner that the inlet
ppm and a mass flow rate 2266.65 kg COD/d. The concentration is equal to the maximum allowable
pinch means the fresh water must be used for mass value) are determined by simultaneously solving the
transfers that take place from the lowest overall material balance and the contaminant material
concentration to a concentration of 2176 ppm. No balance equations (Eqs. 4 and 5) (Prakash and
fresh water is needed in operations taking place at Shenoy, 2005).

2438
 Process integration in the bleaching section of a paper mill for minimization of fresh water consumption and wastewater generation

Table 3. Calculation of the limiting flow rate without considering water loss

Cl2-Washer Alkali Hypo-I mi mk,tot

Conc. Conc. (COD) Fk
3702 Washer Washer
Interval k mgl-1 t/d
t/d 747 t/d 648 t/d
1 30 0 0 0

2 983 0 0
351.69
3 1078
182.70 351.69 335.58
4 1120
356.79 534.39 490.27
5 1190 1375.47
597.6 891.18 768.26
6 2176
2266.65 1056.22
7 2976
2864.25 972.25

FSk,Dp + FS(k+1),Dp = FDp (4) (fresh water) and the remaining 763.32 t/d was
fulfilled by effluent from the hypo washer (S2) and
FSk,Dp * CSk+ F S(k+1),Dp*CS(k+1) = FDp,*CDp (5) alkali washer (S3). Demand for the alkali washer
(D3) was 1930 t/d that has a 1120 ppm COD
If the flow rates obtained by solving the two concentration. To fulfill the demand, only 452.32 t/d
equations are less than the available flow rates of the water from the alkali stage (S3) and 839.86 t/d (fresh
sources, then the demand can be met by these two water) S0 is available. The remaining 637.82 t/d
sources using the calculated flow rates. However, if water can be provided as fresh water or from any
one of these flow rates is greater than the available other source with a COD ≤ 2976 ppm can be used
flow rate (say, FSk,Dp is greater than FSk), then source from other outlets. Thus the minimum water target
Sk is completely used and source S(k − 1) is calculated by the NNA is 3531 t/d.
considered to fulfill the remaining requirement.
Similarly, if FS(k+1),Dp is greater than FS(k+1), then 5. Results and discussion
source S(k + 1) is entirely used and source S(k + 2) is
considered to satisfy the remaining demand. In After designing the water network (Fig. 2) on
general, if Ss is the cleanest source to be used and St the basis of the minimum fresh water requirement, it
is the dirtiest source to be used, then the required was found that the minimum 3531 t/d fresh water
flow rates of Ss and St for the demand Dp are given supply should be maintained in all three operations,
by (Eqs. 6-7): after further distribution of fresh water requirements
of 1028.64 t/d was needed for the chlorine washer,
FSs,Dp + FSt,Dp = FDp – ∑FSi,Dp (6) 1024.68 t/d was needed for the hypo washer and
1477.68 t/d was needed for the alkaline washer. The
FSs,Dp * CSs+ F St,Dp*CSt = FDp,*CDp – ∑ FSi,Dp*CSi total amount of wastewater coming from the chlorine
(7) washer could be recycled in the chlorine washer itself
and the remaining 179.36 t/d could be fulfilled by
Summation for the last term in Eqs. (6) and effluent from the hypo washer. Similarly, the
(7) is i = (s + 1) to (t –1). The NNA is now applied to remaining need of water after fresh water addition in
design the network presented in Fig. 2. In the present the hypo washer can be fulfilled by effluent from the
problem, the minimum water target was calculated hypo washer and effluent from the alkali washer.
by Mann (1999) method. After satisfying the demand of these two washers,
With demand D1 for the chlorination washer only 452.32 t/d effluent remained to be supplied to
containment concentration of 30 ppm COD, the the alkali washer, after that the minimum fresh
nearest neighbor sources were S0 (fresh water) and requirement for the alkali washer was 1477.68 t/d.
S1 (chlorination washer outlet). Eqs. (4) and (5) were Because the amount of available recyclable water
solved to obtain the D1 flow rate (4910 t/d). was insufficient to fulfill the requirement of the alkali
However, the calculated flow rate for S1 (3881 t/d) washer, there is a possibility of taking the desired
was more than the available amount (3702 t/d), so the quality of recyclable water from other outlets.
remaining demand water of D1 was calculated on the However, the minimum water target on the basis of
basis of Eqs. (6) and (7) (179.36 t/d) and was the mass problem table and adjusted with the Mann
fulfilled from the S2 outlet of the hypo washer. (1999) method for water loss was calculated to be
Similarly, demand for the hypo stage, D2 was 1788 2893.18 t/d. The difference may be due to the fact
t/d out of which 1024.68 t/d was fulfilled by S0 that the problem is a fixed load problem and

2439
 Shukla et al./Environmental Engineering and Management Journal 12 (2013), 12, 2435-2442

opportunities exist for demand from the fixed flow total addition of fresh water was calculated to be
rate problem to fulfill the fixed contaminant load 3531 t/d, out of which process waters existing in the
problem. In the existing system, the fresh water system for maintaining the desired consistency
addition was 3831 t/d. However, it includes process account for 2391 t/d. Hence, after applying the NNA
waters existing in the system for maintaining the algorithm, the fresh water requirement was reduced
desired consistency of the pulp leaving washer (oven from 1440 t/d to 1140 t/d. Thus the fresh water
dry pulp to pulp slurry ratio), accounting for 2391 t/d. savings will be about 20. 83 %. Process flow diagram
Therefore, effective fresh water demand is only 1440 of bleaching section after process integration is
t/d in all washers. After designing the network, the presented in Fig. 3.

Fig. 2.Water network for an integrated paper mill developed by using the NNA method

Fig. 3. Process flow diagram of bleaching section after process integration

2440
 Process integration in the bleaching section of a paper mill for minimization of fresh water consumption and wastewater generation

6. Conclusions Bagajewicz M.J., Savelski M.J., (2001), On the use of

linear models for the design of water utilization
The process integration approach is a systems in process plants with a single contaminant,
powerful tool for water conservation in the paper Chemical Engineering Research and Design (Part A),
79, 600–610.
industry, as described in this case study. Paper mills Castro P., Matos H., Fernandes M. C., Nunes C. P., (1999),
consume huge amounts of water and thus present Improvements for Mass-exchange Networks Design,
opportunities for applying the water-pinch approach Chemical Engineering Science, 54, 1649– 1665.
for water conservation. A water targeting problem in Chiang C.L., Hul S., Ng D.K.S., Tan R.R., Foo D.C.Y.,
a paper mill is typical since it is a combination of a (2006), A linear programming model for Retrofit a
fixed load and a fixed flow rate problem. Paper Mill Plant, The Symposium on Process System
Wastewater/process water of various sections are Engineering, Taipei, Taiwan.
characterized by different chemical characteristics Delgado B.E.P.C., Queiroz E.M., Pessoa F.L.P., (2006),
Application of water source diagram (WSD)
like pH, COD, AOX, TDS and color, which can be
procedure in the pulp and paper industry, The Ninth
used as targeted impurities in the water targeting Conference on Process Integration, Modeling and
problem. In the present problem, water targeting was Optimisation for Energy Saving and Pollution
conducted as a fixed contaminant problem and the Reduction (PRES 2006) in conjunction with 17th
water network was designed using the NNA International Congress of Chemical and Process
algorithm for the bleaching section by taking COD as Engineering (CHISA), Praha, Czech Republic.
the target impurity. After developing the target Dhole V.R., Ramchandani N., Tainsh R.A., Wasilewski
network, fresh water was reduced by 20. 83 % in the M., (1996), Make your process water pay for itself,
bleaching section. Application of the fixed Chemical Engineering, 103, 100–103.
Dunn R.F., Wenzel H., (2001), Process integration design
contaminant technique results in a net deficit of
methods for water conservation and wastewater
water; hence, it is not appropriate to apply fixed reduction in industry. Part 1: Design for single
contaminant techniques for a hybrid problem. Before contaminants, Clean Products and Processes, 3, 307–
closing the water stream at the mill level, the water 318.
network needs to be designed on the basis of other El-Halwagi M.M., (1997), Pollution prevention through
impurities like AOX, color, pH and TDS. Cost process integration: systematic design tools, Academic
optimization should be done before applying this Press, San Diego.
technique in the mill. It is clear from the present El-Halwagi M.M., Gabriel F., Harell D., (2003), Rigorous
study that it is possible to recycle wastewater in the graphical targeting for resource conservation via
material recycle/reuse networks, Industrial &
bleaching sections of paper mills. Effects of
Engineering Chemical Research, 42, 4319–4328.
wastewater recycling in the product quality and in the El-Halwagi M.M., El-Halwagi A.M., Manousiouthakis V.,
corrosion of water pipe line should also be studied (1992), Optimal design of dephenolization networks
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Saharanpur for providing data and samples for the present Institute of Chemical Engineers, Part A, 84, 645–651.
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