Article 1

Treatment of Fish Processing Wastewater Using Polyelectrolyte 2

and Palm Anguish 3

Salam K. Al-Dawery 1, Ghadeer E. AL-Yaqoubi 1, Ahoud A. Al-Musharrafi 1, Hamed N. Harharah 2,*, Abdelfattah 4
Amari 2 and Ramzi H. Harharah 2 5

1 Chemical Engineering Department, College of Engineering, University of Nizwa, PC 616, POB 33, Nizwa- 6
Sultanate of Oman; salam@unizwa.edu.om (S.K.A.); 11447688@uofn.edu.om (G.E.A.); 7
11831824@uofn.edu.om (A.A.A.) 8
2 Chemical Engineering Department, College of Engineering, King Khalid University, Abha 61421, Saudi 9
Arabia; hhharharah@kku.edu.sa (H.N.H.); abdelfattah.amari@enig.rnu.tn (A.F.A); ramzi0644@hotmail.com 10
(R.H.H.). 11
* Correspondence: ramzi0644@hotmail.com 12

Abstract: Fish process wastewater has a huge amount of suspended organics, phosphorus and ni- 13
trate that causes environmental damage. This project was designed to treat two types of fish 14
wastewater by applying both chemical treatments using positive and negative and mixed polyelec- 15
trolyte (SNF) with different concentrations (25, 50 and 75 ppm) and physical adsorption using nat- 16
ural material. Several natural materials were selected: Ocimum leaves, Boswellia Scara leaves, Al- 17
Shakher leaves, Tephrosia leaves, Neem leaves, Mentha leaves, Jand peel, Neem Wood, Ocimum 18
fruit, Olive fruit peel and Palm anguish for the treatment of the fish wastewater. The initial tests 19
indicated that the best material was palm anguish. The selected material was treated with 1 M of 20
NaOH solution. Palm anguish was applied at different bed heights (10, 20 and 30 cm). Both, poly- 21
electrolyte, and physical adsorption treatments showed positive impacts on reducing turbidity, con- 22
ductivity, and pH. The level of turbidity was reduced by 50% when using positive polyelectrolyte, 23
and by 30% when using both polyelectrolytes. The conductivity was reduced by 50% and pH was 24
reduced from 8 to 7.2. The use of physical adsorption showed 80% and 85% reduction in the turbid- 25
ity of both types of fish wastewater, especially with a bed height of 30 cm for palm anguish non- 26
washed and treated with NaOH respectively. The use of physical adsorption has a larger impact on 27
treatment compared to that of using polyelectrolyte. 28

Keywords: fish wastewater; polyelectrolyte; palm anguish. 29

Citation: To be added by editorial 30
staff during production.

Academic Editor: Firstname Last-

name 1. Introduction 31
The worldwide production of fish and seafood has increased steadily and trend over 32
Received: date
Revised: date
the last decade which is expected to continue [1]. The fish industries consume large 33

Accepted: date
Published: date
Copyright: © 2023 by the authors.
Submitted for possible open access
amounts of water for washing and cleaning the fish raw materials and processing, conse- 34
quently, resulting in equally large quantities of wastewater [2]. To prevent environmental 35
damage, fish processing wastewater requires treatment before disposal. This effluent con- 36
sists of high contents of organic matter and oil and salt. In principle, these pollutants make 37
their treatment very much difficult [3]. The normal performance of treatment processes of 38
fish processing wastewater within the wastewater treatment plants includes physico- 39

publication under the terms and chemical treatments as primary units for the removal of oils and the particulate matter 40
conditions of the Creative Commons followed by biological reactors (oxidation basin) for the removal of dissolved organic ma- 41
Attribution (CC BY) license terials with the aid of activated sludge [4]. The conventional treatment using activated 42
(https://creativecommons.org/license sludge (CAS) systems are widely employed to treat both industrial and urban wastewater 43
s/by/4.0/). because of their adaptability. 44

Polymers 2023, 15, x. https://doi.org/10.3390/xxxxx www.mdpi.com/journal/polymers

Polymers 2023, 15, x FOR PEER REVIEW 2 of 13

There are many wastewater problems that are faced day by day worldwide. One of 45
the current solutions is traditional sewage wastewater treatment [5]. The different types 46
of fresh wastewater in terms of quality and quantity are not satisfactory because of the 47
high liquid pollutants that come from sewage and the huge increase in the population. 48
Also, waste loading in the fish processing effluents are the major potential source of haz- 49
ards to the coastline and seashore environments [6]. This litter carries different types of 50
bacteria which are a source of many diseases affecting freshwater environments. It also 51
mainly modifies the chemical and biological properties of the receiving ecosystem in the 52
wastewater treatment plant [7,8]. It is one of the most common problems around the world 53
being scrutinized due to the many dangers it has diverged from and resulted from. Cer- 54
tainly, international studies and statistics estimated the global wastewater production 55
is 359.4×109 m3/day, of which only 63 % is collected but 52 % is treated [9]. Almost 30% of 56
global wastewater is produced from fish canning and other fish productions [6]. 57
To shed light on the Sultanate of Oman as a part of the global sewerage systems, 58
studies have indicated that in the year 2000, the production of wastewater was about 59
37.446×106 m3 /year. At the same time, the government in Oman is ramping up investment 60
in the treatment of wastewater and the possibility of reused capacity. Modern technology 61
for sewage collection and disposal infrastructures are established which cover more than 62
98% of urban and rural communities as of 2018. In 2019, more than 68 sewage treatment 63
plant produce about 97 x106 m3/year of treated wastewater. 61% of the produced treated 64
volume is used for agriculture and injection in costa aquifers [10]. There are currently 65
more than 402 treatment plants in the Sultanate, which came in the text of Ministerial Law 66
No. 31/2002, in which it was decided to establish a treatment and management system for 67
sewage collection on December 17, 2002. Subsequently, all stations were included in the 68
same direction and under one name, which is (Haya Water). By the end of 2011, the sta- 69
tions recorded about 84,144 m3/day as a general average collected from sewage, which is 70
expected to rise by 2025 to reach an average volume of 327,853 m3/day [11]. Based on the 71
issue of sewage water around the world and the Sultanate of Oman in particular, and the 72
statistics based on this, fish water is one of the major wastes, whose percentage is increas- 73
ing dramatically and rapidly. The reason behind this is that fish products constitute the 74
largest sectors of global food trade, which is estimated at 78% of the marine products of- 75
fered to global trade competition. 76
In 2010, according to data from the National Institute of Statistics, prepared and 77
canned fish [12,13]. The essential environmental trouble of the fisheries industries in com- 78
mon is the high consumption of water and the maximum productivity of the organic com- 79
ponents, oil and salt contents that flow into the wastewater. Fish processing in many man- 80
ufacturing industries produces massive amounts of wastewater. The production of this 81
wastewater typically consists of producing unwanted parts from the fish such as: properly 82
washing the excess salt, blood, scales, head and entrails, which are not to be typically used 83
as food. The operations of washing, cleaning, cooling, packing and packaging fish con- 84
tribute to an increase in the volume of production of liquid waste, which generates mas- 85
sive quantities of oils, grease, organic materials, salts and others that it brings. In this man- 86
ner, it is formidable to treat due to its high content of these wastes and its subjection to 87
pretreatment in the sewage system and further treatment in the sewerage plant itself. Most 88
countries have tended to put in place measures about this specific type of pollution that 89
fish factories produce to reduce the volume of liquid waste, eliminate it, reduce it, or value 90
the hazardous materials coming from it so that the water efficiency is increased to achieve 91
to obtain water with quality requirements allowed to be used and re-used. Recovering 92
them for other industrial processes in line with economic and environmental sustainabil- 93
ity [14]. 94
Chowdhury et. al. [15]. Stated there is a specific need to put in place rigid regulations 95
for effluent water day after day because rational biological treatment is the best solution 96
for it. The water consumed in the manufacture and processing of fish has become 97
Polymers 2023, 15, x FOR PEER REVIEW 3 of 13

excessive in wastewater, which has shifted it into a primary concern all over the world. 98
The anaerobic flow processes of the Sludge Blanket Reactor (UASB), the Anaerobic Filter 99
(AF) and the Anaerobic Fluid Bed Reactor (AFB), these processes contributed to achieving 100
rapid rates of removal of organic elements and the production of biogases, which were 101
estimated between (80-90%). In addition to these processes, biological conductors, drip 102
filters, and lakes are considered the most suitable medium for the removal of organic ele- 103
ments. The most efficient option for treating wastewater from fish obtain anaerobic drill- 104
ing, followed directly by aerobic drilling. 105
Beltran-Heredia et.al. [16]. studies the development of coagulant agent for treating 106
wastewater. The new coagulant is based on tannin by using Acacia mearnsii de Wild tan- 107
nin extract, NH4Cl and formaldehyde. This coagulant (cationic coagulant) is affected by 108
temperature and tannin–NH4Cl ratio. An ideal combination was found for a ratio of 109
NH4Cl and temperature for each system, 24.9 °C and 2 g/g for dye removal and 36.4 °C 110
and 1.87 g/g for surfactant elimination. the best circumstances were combined to create a 111
combination coagulant that tested on wastewater and surface river water. Its efficacy has 112
been confirmed. 113
Thakur and Choubey [17] presented a study using a natural coagulant (tannin). Nat- 114
ural sources of tannins have been found, leaves, fruits, barks, roots and wood of trees. A 115
substance was extracted and ground from the bark of acacia catechu. To assess coagulant 116
rate and dose, measured turbidity, pH of surface water samples were assessed before and 117
after the jar-test. Also, determine the total suspended solids using the gravimetric method. 118
acacia catechu powder is an effective natural coagulant as it can remove turbidity by 91%. 119
As well as it removes total dissolved solids by 57.3%. 120
Mseddia et.al. [18] carried out a study to reduce the organic load of saltwater from 121
fish industries by optimizing the use of coagulation and flocculation. The results of this 122
study show that the treatment achieved a reduction of 60% of COD and 84% of turbidity. 123
The next step in this process is to treat the effluent by inoculating it with the halophilic 124
consortium. This method involves inoculating the effluent with high concentrations of 125
salts. The results of this study revealed that the combination of biological and physico- 126
chemical treatment resulted in high-performance degradation. 127
De melo and Naval [19] carried out a study aimed to find a different method of tech- 128
nologies that might give massive efficiency of swages treatment and be possible to reuse. 129
For the fish processing industry, there are many difficulties faced in the treatment such as 130
the high concentration of organic materials, suspended solids and the non-uniform con- 131
figuration of the compound. Until this is done, treatment systems are used to scan the 132
sewage and check for pH, TSS, BOD, COD, TN and TP, oils and greases. The comparison 133
found results in concentrations where multiple processes were combined using advanced 134
techniques in treatment, when the goals is reuse or recycling, it achieves the values spec- 135
ified by the industrial reuse criteria. In this study, there was looking to remove important 136
characteristic factors, after mads some analytical comparisons between the different sew- 137
age treatment technologies which involved two different systems conventional and ad- 138
vanced. The factors are pH, TSS, BOD, COD, TN and TP, oils and greases that where treat 139
is focusing on physical treatment as sediment, combining between sediment/decant, 140
float/sediment, and chemical treatment as coagulation/flocculation process, chemical floc- 141
culate, ozone process, oxidation process as adsorb and advanced. Biochemical as: active 142
sludge, filter/anaerobic, bioreactor, aerobic reactor. For further reuse or recycling the 143
treated sewage uses one or more of these technologies and is comprised with quality 144
which determine by the regulations of industrial recycling. 145
Tatiane et.al. [20] presented the treatment of Fish Processing using the coagula- 146
tion/flocculation (C/F) process, by using an organic coagulant (Tanfloc SH) and inorganic 147
coagulant (FeCl3) in the presence of copolymer. These experiments found that the effec- 148
tiveness of Tanfloc SH is the same as that of FeCl3 in treatment fish processing, but natural 149
coagulant is more viable because of the disadvantages of acidification of final supernatant 150
Polymers 2023, 15, x FOR PEER REVIEW 4 of 13

and chemical residues left by inorganic coagulant. The effectiveness of both coagulants 151
was determined by measured color, turbidity removals and COD removal, the COD re- 152
moval data suggest that the C/F process performed well. 153
Hong Anh et al. [21] stated that the considerable increase in wastewater after the use 154
of seawater in the manufacture and treatment of fish and shellfish led to a rapid boom in 155
aquaculture projects, and the annual production in 2018 reached about 94.6 million tons. 156
Total suspended solids (TSS), chemical oxygen demand (COD), biochemical oxygen de- 157
mand (BOD), and modern nitrogen (TN) are identified as the most standard components 158
produced in fish wastewater. To follow the environmental regulations, a giant treatment 159
may be required before discharging, due to the unmoderated concentrations of nutrients, 160
natural compounds and total nitrogen that this water contains. The pH ranges in treating 161
fish effluents with condensate production from 9 to 10, thus, pH is used as a characteriza- 162
tion factor for the emission of ammonia compounds in effluent pollution. The be-around 163
TSS was 635 mg for each liter in addition it was established in one more report that it 164
contributes to an augment in BOD and COD plus total nitrogen levels. The total of one 165
hundred of solids were about 10-30% suspended in the water streaming as of fish 166
wastewater proper to the attendance of proteins and fats. The dissolvable solids vary be- 167
tween 150 to 1,100 mg or even in some cases to even 22,910 mg in fish processing vegeta- 168
tion. The organic composites that are produced from the treatment of fish wastewater hold 169
significant percentages of BOD and COD. They found that the ratios of both differ in fish 170
processing plants and range from about (From 1.1: 1 to 3: 1). Its levels should be reduced 171
by 83 and 66%, respectively, for BOD and COD. Also, their results showed that the percent 172
of nitrogen and phosphorous concentrations vary according to the quality and quantity 173
of fish treated in the wastewater, and this may be due to the amounts of protein contained, 174
and the percentage of nitrogen reaches between (15-20%). This elevated level of ammonia 175
is explained by the presence of slime and blood in the sewage streams. Also, phosphorous 176
has very massive effects, which are produced by processing and cleaning fish, with a vol- 177
ume between 13-47 mg/L. 178
Recently, Priya et al [22] carried out a study for the immobilized thermo-stable en- 179
zyme treated with fish processing wastewater. The treated wastewater was characterized 180
for various parameters such as pH, COD, lipid, and temperature. The optimized operating 181
conditions were found to be 45 °C and 4 hr. The effluent including hydrolyzed fish oil was 182
then treated in a fluidized immobilized carbon catalytic oxidation reactor. When com- 183
pared to the raw water properties, the concentration of each parameter gradually de- 184
creases. This is due to the presence of rice as a catalyst that controls the physical and chem- 185
ical parameters. 186
The objectives of the work are the treatment of fish processing water using positive 187
and negative polyelectrolyte (SFN) as flocculated and investigate the treatment of fish 188
processing water using palm anguish (untreated and treated with NaOH) as a natural 189
adsorbent. 190

2. Materials and Methods 191

For the selecting of natural biomaterials as adsorbent, several natural materials were 192
selected: Ocimum leaves, Boswellia Scara leaves, Al-Shakher leaves, Tephrosia leaves, 193
Neem leaves, Mentha leaves, Jand peel, Neem Wood, Ocimum fruit, Olive fruit peel and 194
Palm anguish. Each of them was dried for 2 days, then grinded and then mix with fish 195
wastewater using Jar tester. The characteristic properties of the sample of fish processing 196
wastewater are: 197
Turbidity (NTU) = 570, 𝜌 = 0.8907 g/ml. 10 g from materials were added to 500 ml 198
of fish wastewater in each beaker of Jar tester. The solutions were mixed at 200 rpm for 199
two min than at 30 rpm for 30 min. samples were collected from each beaker after 1 hr for 200
turbidity analysis. The results are presented in Table 1. Images of settled treated fish 201
Polymers 2023, 15, x FOR PEER REVIEW 5 of 13

wastewater are shown in Figure 1. It can be seen that palm anguish was the best bio- 202
material for adsorption treatment, turbidity was reduced by 90%. 203

Table 1. Natural biomaterial. 204

Plant Sample Turbidity (NTU)

Ocimum leaves 533
Boswellia Scara leaves 289
Al-Shakher leaves 313
Tephrosia leaves 510
Neem leaves 500
Mentha leaves 319
Jand peel 90.8
Neem Wood 91.4
Ocimum fruit 228
Olive fruit peel 198
Palm anguish 61.5
205

206
207

208
Figure 1. Settled treated fish wastewater using natural biomaterials. 209

Two types of experimental tests were carried out for the treatment of fish processing 210
wastewater. 211
1. Chemical treatment using polyelectrolyte. 212
2. Physical adsorption using palm anguish. 213
Polymers 2023, 15, x FOR PEER REVIEW 6 of 13

Two samples of fish processing wastewater were collected from the Nizwa fish mar- 214
ket with different characteristics as shown in Table 2. 215

Table 2. Characteristics of samples of fish wastewater. 216

Sample Turbidity pH Conductivity (ms/cm)

1 44.7 7.88 767
2 79.3 7.95 755
217
Two types of polyelectrolytes were used: positive and negative SNF as flocculents 218
for the treatment of fish processing wastewater. 1 gram of each polyelectrolyte was dis- 219
solved gradually in 1 liter of distilled water and then stirred for 24 hr using a magnetic 220
stirrer. Jar tester was used for mixing different concentrations of polyelectrolytes with 1 L 221
of fish process water filled in 6 beakers with fish wastewater (blood), each beaker with 1 222
L and adding a different volume of positive and negative polyelectrolyte into each beaker 223
(25, 50 and 75 mL). The solutions were mixed at 200 rpm for 2 min for proper mixing and 224
then mixed at 30 rpm for 30 min to allow for flocculation. The solution of each beaker was 225
poured into a graduated cylinder and during settling, samples of supernatant were col- 226
lected each 30 min for analysis (turbidity, pH, conductivity). 227
For natural adsorption, palm anguish was selected as natural adsorption for the treat- 228
ment of fish processing wastewater. Palm anguish was collected from a local farm. The 229
palm anguish was grinded are then sieved; the selected grinded size was 500-710 µ m. To 230
enhance the adsorption capacity, the grinded palm anguish and 83 g of palm anguish were 231
soaked in 2 L of 1 N NaOH for 24 hours. Then the anguish was filtered and washed several 232
times with distilled water until the pH reduce to 7. The solid was dried in an electrical 233
oven at 60 °C for 24 hours. 3.5 FTIR for palm anguish adsorbent. The characteristic com- 234
position of both anguish samples (treated with NaOH and non-treated) were analyzed 235
using FTIR at Daris laboratory at the University of Nizwa. The results of FTIR are shown 236
in Figure 2. The positions of the most characteristic bands for lignin in the region are 1585 237
cm-1 for aromatic skeletal vibrations, 1415 cm-1 for C-H deformation, 1315 cm-1 for sy- 238
ringyl ring plus guaiacyl ring, and 1112 cm-1 for aromatic skeletal vibrations. Usually, a 239
broad peak between 3000 to 3500 reflects the presence of OH functional group or NH 240
functional group. A FTIR peak at 1030 reflects either S=O stretching of sulfoxide functional 241
group or CO-O-CO stretching of anhydride. 242
243

Without NaOH
With NaOH
Internsity (a.u.)

1029.93217

1585.40121 2358.8147
1415.67456
1313.45283 3330.88552

1109.1543

555.46904 1028.00346

500 1000 1500 2000 2500 3000 3500 4000

-1
Wavenumber (cm )
244
Figure 2. FTIR analysis of palm anguish, treated and non-treated with NaOH. 245
Polymers 2023, 15, x FOR PEER REVIEW 7 of 13

The adsorption process using treated and non-treated palm anguish with NaOH and 246
performed in a cylindrical column with a height of 100 cm and a diameter of 2.8 cm. The 247
experimental photo and schematic diagram are depicted in Figure 3. Bed height of palm 248
anguish was used (10 cm, 20 cm, and 30 cm). The fish wastewater was pumped through 249
the column using a dozing pump (china-YZ1516x-Baoding Chuangrui Precision Pump 250
Co. Ltd) with a flow rate ranging from 0.0064 L/min to 0.021 L/min. Samples from the 251
outlet were collected every 5 minutes until anguish was saturated. 252

During the experiment, the selected flow rate of fish wastewater through the beds was 253
0.0142 L/min using a peristaltic pump at a speed of 20 rpm. 254

(a) (b)
Figure 3. (a) Adsorption process (b) Schematic diagram. 255

3. Results 256

3.1. Results of treated fish wastewater using polyelectrolyte 257

For the chemical treatment of the two types of fish processing wastewater, different 258
concentrations (25 mL, 50 mL, 75 mL) of positive and negative polyelectrolytes were used. 259
The results of turbidity, pH and conductivities are shown in Figures 4-6 for the treatment 260
of sample 1 and Figures 7-9 for the treatment of sample 2. The results of using mixed 261
polymer are shown in Figures 10-12. The results showed a positive impact of using posi- 262
tive polyelectrolyte on turbidity in the fish wastewater, the maximum reduction in tur- 263
bidity was reached 50 % by adding 25 mL on sample 1, see Figure 4a, while excessive 264
addition of polyelectrolyte has less effect on turbidity due to repulsion between polyelec- 265
trolyte particles of similar charges as the concentration increased. Turbidity was reduced 266
by 30 % when adding 50 mL, but not much change in turbidity when adding 75 mL. For 267
using negative polyelectrolyte, turbidity was reduced by 25% by adding 25 mL, see Figure 268
4b, while excessive addition of polymer has not much effect on turbidity. This behavior 269
may be referred to as the repulsion between negative polymer charge particles and the 270
inorganic phosphate (𝑃𝑂3− ) and Nitrate (𝑁𝑂2− )that present in the wastewater. Also, the 271
better reduction of turbidity using positive polyelectrolyte may be due to the reaction of 272
inorganic and organic phosphate-suspended materials and hence leading to the precipi- 273
tation of these materials and reducing turbidity. 274
Polymers 2023, 15, x FOR PEER REVIEW 8 of 13

It can be seen a little drop in pH value as shown in Figure 5. This may be due to a 275
reduction in carboxylic ions as reacted with positive polyelectrolyte as well as a reduction 276
of positively charge carbonyl groups using negative polyelectrolyte. Also, the results 277
showed that the conductivity (Figure 6) was reduced by almost 50% when using both 278
negative and positive polymers. This reduction could be due to the precipitation of dis- 279
solved metal contents using polyelectrolytes with opposite charges and orthophosphate 280
and calcium bicarbonate that reacted with both positive polyelectrolyte and negative 281
polyelectrolyte respectively. 282

(a) (b)
Figure 4. Turbidity of treated fish wastewater (sample 1) using (a) positive polyelectrolyte; (b) neg- 283
ative polyelectrolyte. 284

(a) (b)
Figure 5. The pH of treated fish wastewater (sample 1) using (a) positive polyelectrolyte; (b) nega- 285
tive polyelectrolyte. 286

(a) (b)
Polymers 2023, 15, x FOR PEER REVIEW 9 of 13

Figure 6. The conductivity of treated fish wastewater (sample 1) using (a) positive polyelectrolyte; 287
(b) negative polyelectrolyte. 288

The results of turbidity of treated sample 2 of fish wastewater, Figure 7, showed a 289
reduction by 50 % using positive polyelectrolyte with all concentrations (25, 50 and 75 290
mL), while the turbidity was reduced by 50% only with using 25 mL of negative polyelec- 291
trolyte and no much change in turbidity when using other amounts. This may be due to 292
repulsion between negative polyelectrolyte with the negatively charged inorganic phos- 293
phate (𝑃𝑂3− ) and Nitrate (𝑁𝑂2− ) that present in wastewater. Comparisons between the 294
treatment of samples 1 and 2 using polyelectrolytes indicates that the effect of the polymer 295
has a larger impact on samples with larger turbidity due to the large chance of attraction 296
between polymer and particles of pollutants that present in the wastewater. 297
It can be seen a little drop in pH value from 7.96 to 7.3 as shown in Figure 8. The 298
reduction in pH may be due to a reduction in carboxylic ions as reacted with positive 299
polyelectrolyte as well as a reduction of positively charge carbonyl groups using negative 300
polyelectrolyte. Like that of sample 1, the conductivity (Figure 9) was reduced by almost 301
50% when using both negative and positive polymers. This reduction could be due to the 302
precipitation of dissolved metal contents using polyelectrolytes with opposite charges and 303
orthophosphate and calcium bicarbonate that reacted with both positive polyelectrolyte 304
and negative polyelectrolyte respectively. 305

(a) (b)
Figure 7. Turbidity of treated fish wastewater (sample 2) using (a) positive polyelectrolyte; (b) neg- 306
ative polyelectrolyte. 307

(a) (b)
Figure 8. The pH of treated fish wastewater (sample 2) using (a) positive polyelectrolyte; (b) nega- 308
tive polyelectrolyte. 309
Polymers 2023, 15, x FOR PEER REVIEW 10 of 13

(a) (b)
Figure 9. The conductivity of treated fish wastewater (sample 2) using (a) positive polyelectrolyte; 310
(b) negative polyelectrolyte. 311

The use of mixed positive and negative polymers reduced turbidity by 50% with 312
mixed polymer concentrations of 50 and 75 mL as shown in Figure 10a. This reduction in 313
turbidity at higher concentrations refers to the increase in the amount of positive poly- 314
electrolyte like that of treated samples 1 and 2. 315
It can be seen a little drop in pH value from 8.2 to 7.1 as shown in Figure 10b. The 316
reduction in pH may be due to the reduction in carboxylic ions as reacted with positive 317
polyelectrolyte as well as the reduction of positively charge carbonyl groups using nega- 318
tive polyelectrolyte. Like that of sample 1, the conductivity in Figure 10c was reduced by 319
almost 40% when using both negative and positive polymers. This reduction could be due 320
to the precipitation of dissolved metal contents using polyelectrolytes with opposite 321
charges and orthophosphate and calcium bicarbonate that reacted with both positive 322
polyelectrolyte and negative polyelectrolyte respectively. 323

Turbidity

50

40
Turbidity

30

20

10 mixed 25ml mixed 50ml mixed 75ml

0
0 20 40 60 80 100 120 140
Time (min)

(a) (b)
Polymers 2023, 15, x FOR PEER REVIEW 11 of 13

(c)
Figure 10. The (a) Turbidity; (b) pH; (c) conductivity of treated fish wastewater (sample 1) using 324
mixed polyelectrolytes. 325

3.2. Results of treated fish wastewater using natural adsorption on sample 1 326

Palm anguish was used as a natural adsorbent for the treatment of fish wastewater. 327
washed with NaOH was used as an adsorbent for the treatment of fish processing 328
wastewater. Three different bed heights were used: 10, 20 and 30 cm. The flow rate of fish 329
wastewater through the beds was 0.0142 L/min using a peristaltic pump at speed of 20 330
rpm. The results are depicted in Figures 11a-b. 331
It can be seen when using a bed of treated Palm anguish with NaOH that using a bed 332
height of 30 cm gave a better result for reducing turbidity compared to other bed heights 333
of 10 and 20 cm, Figure 11a. The break time using the three-bed heights 10, 20 and 30 cm 334
are 170, 250 and 370 min respectively. It is clear that the break time point of the bed with 335
30 cm is much longer than others. The bed height of 30 cm provides an opportunity for 336
the adsorption process of the pollutants present in the fish water. The palm anguish is 337
washed with NaOH which in turn expands the pores so that the adsorption process of 338
pollutants takes place more and prevents them from falling with the outputs. 339
The results of using untreated palm anguish NaOH are depicted in Figure 11b. It can 340
be observed that using bed heights of 20 and 30 cm gave almost similar and better results 341
compared to those obtained results using a bed height of 10 cm. Both beds 20 and 30 cm 342
have a break time of 250 and 300 min respectively, while 10 cm has a break time of 230 343
min. 344

(a) (b)
Polymers 2023, 15, x FOR PEER REVIEW 12 of 13

Figure 11. Turbidity of adsorption process using untreated palm anguish (a) with NaOH; (b) with- 345
out NaOH. 346

The pH and conductivity results from the adsorption process showed a reduction 347
of 0.8 in pH level and 42% in conductivity of fish wastewater as depicted in Table 3. The 348
reduction in conductivity refers to the adsorption of ion metals onto the surface of palm 349
anguish, especially with that treated with NaOH due to the availability of pore surface 350
area. 351

Table 3. Results of the pH and conductivity of treated fish wastewater using pal anguish. 352

Initial conductivity Final conductivity

Palm anguish Initial pH Final pH
(ms/cm) (ms/cm)
Treated with
7.88 7.2 767 322
NaOH
Non-treated 7.88 7.35 767 354

4. Conclusions 353
Throughout the experimental works, it was found that the chemical treatment using 354
positive and negative polyelectrolytes gave a good reduction in the turbidity of fish 355
wastewater reaching 50 %. There was a 50 % reduction in conductivities and pH was re- 356
duced from 8 to 7. The results of physical adsorption using treated and untreated palm 357
anguish treated with NaOH showed a sufficient reduction in the turbidity reaching 85 % 358
and a break time of 370 minutes using a bed height of 30 cm of treated palm anguish. 359
Conductivity was reduced by 42 % with adsorption using treated palm with NaOH, but 360
there was a small reduction in pH. These results showed that treating fish wastewater 361
using physical adsorption is more sufficient compared to that using chemical treatment. 362
Conductivity and pH were reduced and little drop in the pH in both positive and 363
negative polyelectrolytes separately as well as for the case of mixing of positive and neg- 364
ative polyelectrolytes. 365
Physical adsorption using original palm anguish as adsorbent positively impacted 366
reducing turbidity, especially at a 30 cm height. 367

Author Contributions: Theory, S.K.A. and G.E.A.; experimental testing, S.K.A. and A.A.A.; model- 368
ling, S.K.A. and A.A.A; drafting, S.K.A. and G.E.A; validation, S.K.A. and H.N.H; editing, R.H.H; 369
supervision, A.F.A. and H.N.H. 370

Funding: This research was funded by the Deanship of Scientific Research at King Khalid University 371
under grant number RGP2/133/44. 372

Data Availability Statement: Not applicable. 373

Acknowledgments: The authors extend their appreciation to the Deanship of Scientific Research at 374
King Khalid University for funding this work through a Large Group Research Project under grant 375
number RGP2/133/44. 376

Conflicts of Interest: The authors declare no conflict of interest. 377

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