Journal of Water Process Engineering 31 (2019) 100809

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Journal of Water Process Engineering

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T
The occurrence of natural organic matter in South African water treatment
plants
Pfano Tshindane, Phumlile P. Mamba, Lerato Moss, Umhle U. Swana, Welldone Moyo,
Machawe M. Motsa, Nhamo Chaukura, Bhekie B. Mamba, Thabo T.I. Nkambule
⁎

Nanotechnology and Water Sustainability (NanoWS) Research Unit, University of South Africa, College of Science Engineering and Technology (CSET), UNISA Science
Campus, 1710 Roodepoort, Johannesburg, South Africa

A R T I C LE I N FO A B S T R A C T

Keywords: Water supplied to customers must be safe and fit for purpose. It is thus important that the water from water
Dissolved organic carbon treatment plants (WTPs) meets World Health Organization standards or local standards such as the South African
Natural organic matter National Standard, before distribution. This study focuses on the treatment of natural organic matter (NOM) in
Water treatment plants South African WTPs. The problems associated with NOM include: (1) it affects the organoleptic properties of
water; (2) increases coagulant demand; (3) reacts with chlorine to form disinfection by-products and (4) causes
membrane fouling. The aim of the study was to characterise the NOM composition of various water sources.
Specifically, the objectives were: (1) to assess the character of NOM in selected regions of South Africa; and (2) to
evaluate the NOM removal efficiencies of the selected WTPs. To achieve these, various characterisation tech-
niques were used to determine parameters such as dissolved organic carbon, ultraviolet absorbance, specific
ultraviolet absorbance, and dissolved organic matter, using fluorescence excitation-emission matrix spectro-
scopy. The character of NOM evolved throughout the treatment process as a result of coagulation, sedimentation
and filtration processes. As indicated by SUVA, a decrease in the hydrophobic fraction of NOM from raw to final
water was observed, except for plant C2 in Region C where a drastic increase in SUVA from 1.26–31.95 L/mg.m
was observed, indicating an increase in the hydrophobic compounds in water. All WTPs were shown to have
different removal efficiencies because of the character of NOM in the raw water and the coagulation conditions
used.

1. Introduction
Safe drinking water is a major concern in developing and water-
scarce countries such as South Africa. Rapid population growth, ex-
tensive industrialisation, and agricultural activities have resulted in the
pollution of water sources (Nkambule et al., 2012). These activities
contribute a wide range of organic and inorganic pollutants in water
sources through surface runoff, point source waste discharges, and
other diffuse (non-point) sources [1]. Natural organic matter (NOM) is
a complex combination of organic compounds formed from the decay of
plant and animal matter in water sources and soil [2], and is one of the
major problematic pollutants found in drinking water sources [3–5].
These organic compounds originate from autochthonous sources
which are created within the water body, and allochthonous sources
which are derived from outside the water body [6]. The composition of
NOM in water sources depends on the geographic and climatic condi-
tions and its character changes throughout the water treatment process
[7,8]. Based on the polarity, NOM is divided into hydrophobic (humic),
hydrophilic (non-humic), and transphilic (intermediate polarity) frac-
tions [9,10]. The hydrophobic fraction consists of humic substances
(HS), which in turn are made up of humic acids (HA), fulvic acids (FA),
and humin [6]. These substances contribute to the yellow-brownish
colour of water, impacting the water quality [11]. The hydrophilic
fraction consists of non-humic substances such as proteins, carbohy-
drates, and polysaccharides [12], while the transphilic fraction is
composed of mainly of carboxylic acids [13].
The presence of NOM in raw water causes numerous problems in
water treatment processes, such as high coagulant dosage, production
of disinfection-by products (DBPs), unpleasant taste, odour and yellow-
brownish colour, membrane fouling and the promotion of bacterial re-
growth in the distribution system since NOM serves as a source of food
for heterotrophic organisms [14–16]; Nkambule et al., 2012). These
problems indicate the need to remove NOM from drinking water sup-
plies.

⁎
Corresponding author.
E-mail address: nkambtt@unisa.ac.za (T.T.I. Nkambule).

https://doi.org/10.1016/j.jwpe.2019.100809

2214-7144/ © 2019 Elsevier Ltd. All rights reserved.

Received 4 October 2018; Received in revised form 13 March 2019; Accepted 21 March 2019
P. Tshindane, et al.
To date, only a few studies on the characterisation and quantifica-
tion of NOM at water treatment plants (WTPs) in South Africa have
reported NOM occurrence at individual WTPs [7,17,9]; Marais et al.,
2018; [5]). These studies assessed the composition of NOM in water
using various parameters such as dissolved organic carbon (DOC),
which gives the quantity of NOM in water, and ultra-violet absorbance
analysis (UVA), which identifies the different chromophores of NOM.
For instance, UV at 254 nm indicates aromaticity, and UV at 272 nm is a
good indicator of DBP formation potential. Specific ultraviolet absor-
bance (SUVA) gives an indication of the amount of humic substances vs.
non-humic substances in NOM [18] in terms of hydrophobic (SUVA
> 4), hydrophilic (SUVA < 2), and transphilic (2 < SUVA < 4)
fractions. Fluorescence excitation-emission matrix (FEEM) spectroscopy
provides information on the structural composition of NOM based on
excitation and emission wavelengths of the fluorophores within NOM.
Most WTPs in South Africa use the conventional treatment process,
with coagulation-flocculation as the major NOM removal processes, and
chlorination as the disinfection process [4]. It is therefore important to
track the nature of NOM at each treatment step to assess the NOM re-
moval efficiency of treatment processes given the diverse types of water
sources in South Africa [4]. This will assist in WTP optimisation, which
will lead to enhanced NOM removal. Due to the diverse nature of South
African fresh water sources, the character of NOM varies and thus it
cannot be effectively removed with only one treatment regime. Thus,
this work sought to develop an understanding of the NOM character in
water treatment plants in a bid to improve NOM removal through
process optimisation. The aim was to characterise the NOM composi-
tion of various water sources, and the objectives were: (1) to assess the
nature, composition and character of NOM in selected regions of South
Africa, and (2) to evaluate the NOM removal efficiency of selected
water treatment plants. The work focused on the individual NOM
fractions in three South African provinces and their removal by dif-
ferent water treatment plants. The study is part of a series of assess-
ments conducted on the same plants over all four seasons, and is re-
presentative of the behaviour of NOM in South African water treatment
plants.
2. Methodology
2.1. Sampling sites
The WTPs selected for this study are located in three regions across
South Africa and are represented by codes (Fig. 1). From Region A,
Fig. 1. The location of the selected water treatment plants in South Africa.
2
Journal of Water Process Engineering 31 (2019) 100809
plants A1, A2, and A3 were sampled, from Region B, plants B1, B2, B3,
and B4 were selected, and from Region C, plants C1 and C2 were
chosen. The treatment processes used in each of the plants are provided
in Table S1.
2.2. Sampling and sample analyses
Sampling at all nine water treatment plants was performed in tri-
plicate. Samples were collected at each of the treatment steps using 1 L
amber glass bottles and stored in a cooler bag. The turbidity, con-
ductivity, and pH were measured onsite using a turbidity meter
(Thermo Scientific Orion AQUAfast® AQ3010), a conductivity meter
(XS Instruments, Carpi, MO, Italy), and a pH meter (XS Instruments,
Carpi MO, Italy), respectively. These parameters were measured to
obtain the physical properties of the water [19]. Dissolved organic
carbon analyses were performed using a Torch Total Organic Carbon
Analyzer (Teledyne Tekmar, Mason, Ohio, USA) after filtering the
samples through a 0.45 μm filter. Dissolved organic carbon (DOC) is the
fraction of total organic carbon that passes through the 0.45 μm filter
[20].
Ultraviolet-visible absorbance analyses were performed using a
fluorescence excitation-emission matrix (FEEM) spectrometer
(Aqualog®, HORIBA Scientific, New Jersey, USA). All samples were
analysed over a full wavelength spectrum (200–800 nm) to effectively
study the NOM character. Particular attention was given to the fol-
lowing wavelengths, which are representative of particular NOM frac-
tions: 214 nm indicates the presence of nitrates and nitrites; 254 nm
indicates the presence of humic substances and aromatics; 272 nm is the
best predictor of the formation of trihalomethanes (THM) [9,15]. Fur-
thermore, it is possible to classify and distinguish humic substances of
various origins using FEEM data (Chen et al., 2003).
The ratio between UV absorbance at 254 nm and DOC is called the
specific ultraviolet absorbance (SUVA) (Equation [1]), and is an in-
dication of the quantity of humic substances in comparison with non-
humic substances in NOM [18].
UV254
SUVA = × 100
DOC (1)
3. Results and discussion
3.1. Physicochemical characteristics of water
Except for plant B1 with final water turbidity of 1.4 NTU, the final
water of all WTPs was found to have a turbidity of < 1 NTU (Fig. 2). A
slight increase in turbidity was observed after the filtration stage for
plants B1 and B2, with values ranging from 0 to 1.4 and 0 to 0.96 NTU,
respectively. This could be due to the breakthrough of the retained
solutes on the Schmutzdecke (“dirt cover”) and the filter bed [21,22].
The Schmutzdecke is a biological layer that builds up on the surface of
the slow sand filter, and facilitates the effective purification in the
treatment of drinking water (Dehwah and Missimer, 2007). All the
WTPs studied use coagulation-flocculation for the removal of turbidity
and color. An increase in turbidity from 0 to 0.2 NTU was observed at
plant C1 following the addition of a coagulant. At plant B2, the increase
in turbidity from 0.6 to 2.7 NTU after sedimentation could be due to the
accumulation of scum on the tanks and floc carryover. A drastic in-
crease in turbidity from 0.3 to 2.7 NTU for the other plants was ob-
served after sedimentation, indicating poor control of the coagulation
process. Turbidity is an indication of the presence of suspended and
colloidal particles in water (Oladoja et al., 2017). Turbidity describes
the amount of light scattered by particles in the water and it can be used
as an indicator of the performance of the coagulation process. The
South African National Standard [23] specifies that the turbidity of the
final water must be less than 1 NTU.
The pH of water is another critical parameter that greatly influences
P. Tshindane, et al. Journal of Water Process Engineering 31 (2019) 100809

Fig. 2. The physicochemical properties of water at different treatment steps for water treatment plants in Regions A, B, and C.

3
P. Tshindane, et al.
Fig. 3. The DOC concentrations in raw water for water treatment plants in Regions A, B, and C.
the quality of produced water, especially during coagulation. The re-
moval of NOM during coagulation is largely influenced by pH [5]. The
final pH of water for the plants ranged from 7.3–9.3, which is within the
[23] specification of pH 5–9.7. The pH for A3 was stable due to no
addition of lime, and there were no major changes in pH for plants A1,
A2 and A3 (Fig. 3). The slight increase in pH for the coastal plants (B3,
B4, C1, and C2) was due to the addition of hydrated lime, which made
the water alkaline. However, the pH decreased after chlorination due to
the formation of hypochlorous ions, which reduced the pH of the water
to acceptable levels.
Another parameter that affects the quality of water is electrical
conductivity, which describes the load of charged species in water [19].
These are a result of dissolved salts and inorganic materials such as
alkalis, chlorides, sulphides and carbonate compounds present in the
water. Raw water conductivity values of > 10 mS/cm, which correlate
to fresh water, were observed at plants A2 and A3. However, there was
a significant increase in conductivity for the feed streams from Regions
B and C, which illustrates the varied types of raw water as influenced by
the geographic locations which subsequently affect the properties of
NOM in the water. The electrical conductivity of all the plants in-
vestigated varied for each plant due to different types and dosage of
coagulants used (Table S1), with the lowest being recorded in plant A1
with a conductivity value approaching 0 mS/m, and the highest con-
ductivity recorded in plant B2 (129 mS/m). Overall, compliance in
terms of the aesthetic limits (2015 Blue Drop Limits) of less than
170 mS/m set by the South African National Standard (SANS) for
Drinking Water [23] was observed for all the plants.
3.2. Dissolved organic carbon
The concentration of DOC in raw water was found to be different for
each treatment plant (Fig. 3) due to the different geographic location of
each plant. For example, plant A1 (DOC = 0.74 mg/L) obtains its raw
water from a dam located on the slopes of mountains, consequently the
plant does not apply sedimentation as a treatment step. It is noteworthy
that the DOC concentration of the final treated water from all WTPs was
4
Journal of Water Process Engineering 31 (2019) 100809
found to be below the limits set by [23], which is ≤10 mg/L. Dissolved
organic carbon analysis alone does not provide adequate information
on the transformation of NOM throughout the treatment process [24].
However, coagulation and flocculation processes are responsible for the
reduction of DOC at WTPs [25].
Despite the largely similar treatment processes in most WTPs (Table
S1), DOC removal efficiencies were found to be different at all WTPs.
These differences can be attributed to the different coagulants and
dosages used during coagulation. Plants in Region C, which use alu-
minium-based salt polymer as a coagulant, have the highest DOC re-
moval efficiency (46.3 and 61.8% for plants C1 and C2, respectively).
Since the treatment processes used by these WTPs are essentially si-
milar to those of other WTPs, the high removal efficiency is likely to be
due to either the NOM character in that region, or the coagulant type
and dosage used, or a combination of these. The aim of further in-
vestigations should be to elucidate the impact of various coagulants on
DOC removal. Laboratory-scale experiments involving jar testing to
optimise pH and coagulant dosage would be a good starting point. The
character of NOM is influenced by the surrounding geology and human
activities [4,26]. Interestingly, there was an increase in DOC content
throughout the treatment process for plants A1, A2, and B4. This could
be due to clogged sand filters or biological degradation occurring on the
edges of the sedimentation tanks as shown by flakes of decomposing
matter that are washed off into the water [27].
3.3. Ultraviolet absorbance
Ultraviolet absorbance (UVA) was measured at a wavelength range
of 200–600 nm. As mentioned before, absorbance at 214 nm represents
nitrites and nitrates while 254 nm represents the aromaticity of NOM,
and absorbance at 272 nm signifies the potential of DBP formation [6].
A decrease in the absorbance at 254 nm was observed from raw
water to final water for all the WTPs (Fig. 4). This result shows that the
aromatic content of the water decreases throughout the treatment
processes. The highest UV254 absorbance (0.47 cm−1) was observed at
plant C2 indicating that the raw water is rich in aromatic compounds.
P. Tshindane, et al.
Fig. 4. Ultraviolet absorbance data for plants in Regions A, B, and C.
The UV214 for raw water of all investigated WTPs is high, indicating the
presence of high levels of nitrates and nitrites. Furthermore, all WTPs
showed high potential for DBP formation as indicated by the high UV272
absorbances.
From these results, the highest percent removal of NOM was ob-
served at plants C1 and C2 with removal efficiencies of 64.3 and 89.4%,
respectively. Low NOM removal efficiencies were observed for the
other WTPs. The difference in removal efficiency is attributable to
different types of water sources and coagulants used in the treatment
processes.
3.4. Specific ultraviolet absorbance
Specific ultraviolet absorbance (SUVA) gives an indication of the
hydrophobicity, transphilic and hydrophilicity of the NOM in the water
[10,28]. A low SUVA value (< 2 L/mg.m) indicates the presence of
mainly hydrophilic fractions of NOM, while a high SUVA value (> 4 L/
mg.m) indicates the presence of mainly hydrophobic fractions of NOM,
and SUVA values of between 2 and 4 L/mg.m indicate the presence of
the transphilic fractions of NOM [5,27].
The SUVA values for raw water in all the plants investigated were
greater than 4 L/mg.m, implying that the raw water consists mainly of
hydrophobic NOM (Table 1). From the results, SUVA values for the final
water treated at plants B4, B2, and A2 were 2.92, 3.06, and 3.19,
5
Journal of Water Process Engineering 31 (2019) 100809
respectively. This indicates that the nature of the NOM found in the
water treated changed to transphilic along the treatment trains. This is
consistent with previous studies that reported transphilic NOM in final
water at a WTP in South Africa [20]. The SUVA values for plants A1 and
B3 were found to increase after coagulation, suggesting the transfor-
mation of NOM into hydrophobic fractions. This result is unexpected
because hydrophobic NOM is more amenable to removal by coagula-
tion [20]. Plants A1 and B3 use Polymer U3800 and Zeta Floc 553,
respectively, as coagulants; however, it seems that these coagulants are
ineffective in removing NOM. The overall trend observed throughout
the plants is that the SUVA values decreased after the raw water was
treated using these different water treatment processes. It should be
noted that NOM is not routinely monitored in WTPs in SA, and, as such,
WTPs do not prioritise its removal. In fact, because its impact is an
emerging area of study, and due to its propensity to form disinfection
by-products (DBPs), NOM and DBPs have been classified as emerging
pollutants [29,30]. However, as demonstrated in Table 1, DOC is pre-
sent even in treated water, albeit at low concentrations (0.79–2.09 mg/
L). It is currently not known what DOC concentrations would offset the
formation of DBPs, thus these concentrations should also be monitored.
3.5. Fluorescence emission excitation matrices
Fluorescence excitation-emission matrix (FEEM) spectroscopy
P. Tshindane, et al. Journal of Water Process Engineering 31 (2019) 100809

Table 1
Chemical properties of water at different treatment stages of the WTPs.
WTP ID DOC (mg/L) UV254 (cm−1) SUVA (L/mg.m)

Raw Coagulation Final Raw Coagulation Final Raw Coagulation Final

A1 0.74 0.65 0.79 0.06 0.63 0.06 7.94 9.70 7.04

A2 1.86 1.93 2.09 0.10 0.09 0.07 5.43 4.95 3.19
A3 1.73 1.59 1.56 0.18 0.10 0.07 10.52 6.52 4.40
B1 2.06 1.03 0.16 0.09 7.93 4.81
B2 1.73 1.97 1.96 0.14 0.10 0.06 8.29 5.03 3.06
B3 1.26 1.08 1.16 0.19 0.17 0.12 14.64 15.34 10.03
B4 1.35 0.99 1.82 0.18 0.06 0.05 13.39 5.89 2.92
C1 2.78 1.45 1.44 0.25 0.12 0.06 9.33 8.26 4.17
C2 2.83 1.95 1.47 0.05 0.11 0.47 1.26 5.82 31.95

Table 2 The FEEM results showed peaks in three regions, namely A, C, and T
Commonly referenced peak and region locations of excitation-emission ma- (Fig. 5) [31]. The spectra demonstrated that the most dominant NOM
trices obtained for aquatic humic substances and dissolved organic matter category is humic-like with excitation wavelengths of between 260 and
([31]). 360 nm and emission wavelengths of between 400 and 460 nm for all
Peak Excitation Emission maximum Description of the plants investigated. However, different excitation/emission wave-
label maximum (nm) (nm) fluorophores lengths were recorded for plant B3, which indicated the presence of
both tryptophan-like and humic-like compounds in raw water ab-
B 275 305 Tyrosine-like, protein
likea
stracted from the river [6,32]. Narrow peaks were observed in the final
T 275 340 Tryptophan-like, water for plants C1, B3, A3 and A2, indicating that the treatment pro-
protein like cess effectively removed HA from the water. Broad peaks were observed
A 260 400-460 Humic-like in the final water of plants C2, B2, B1, A1 and B4, indicating that the
M 290-310 370-410 Marine humic-like
treatment process is ineffective for the complete removal of HA in the
C 320-360 420-460 Humic-like
D 390 509 Soil fulvic acid water [33]. Overall, there is a clear trend that the intensity of the peaks
E 455 521 Soil fulvic acid declines as the water moves through the treatment process, suggesting
N 280 370 Plankton derived that the NOM content was reduced.
As predicted by Equation 1, an increase in DOC and a decrease in
UVA resulted in a decrease in SUVA. However, for plants A3, C1, B3,
provides information on the structural composition of NOM based on and B1 the trend was found to be inconsistent. Further research would
the excitation and emission wavelength of the fluorophores (Table 2), be required to investigate this discrepancy. From FEEM spectra, there is
and the absorption wavelengths, together with the assigned com- a monotonic waning of the peaks, indicating a progressive decline in
pounds, are derived from current guidelines based on previous studies NOM along the treatment train. The same general trend is shown for
[31]. DOC.

Fig. 5. Fluorescence excitation-emission matrix spectra for water samples collected in (a) C1, (b) C2, (c) B2, (d) B3, (e) B1, (f) B4, (g) A3, (h) A1, and (i) A2 WTPs.

6
P. Tshindane, et al.
4. Conclusion
This work sought to develop an understanding of the NOM character
in selected water treatment plants in South Africa in a bid to improve
NOM removal through process optimisation. The aim was to char-
acterise the NOM composition of various water sources in South Africa.
The study demonstrated that NOM undergoes transformation as the
water traverses through the treatment train. This was shown by the
changing hydrophobicity of NOM along the treatment train. Through
SUVA, it was observed that NOM generally becomes less hydrophobic
after coagulation and flocculation processes. However, the major lim-
itation of the current approach is that the characterisation methods do
not provide adequate information about the evolving chemical char-
acter of NOM. Techniques based on molecular weight distribution, and/
or more advanced approaches such as the polarity rapid assessment
method (PRAM), or liquid chromatography coupled with organic
carbon detection (LC-OCD), would be useful in future studies. The re-
moval of NOM using conventional treatment processes has been re-
ported to depend on the character of NOM, which in turn is influenced
by its origin. The highest DOC removal efficiency was observed at plant
C2. Negative DOC removal efficiencies were observed at plants A1, A2,
and B4 due to either clogged filters, or the biological activity on the
edges of the sedimentation tanks. An increase in DOC was accompanied
by a decrease in UVA and SUVA for most plants. However, for plants
A3, B1, B3, and C1 the trend was inconsistent. Further research would
be required to investigate this discrepancy.
Although all the WTPs studied used the conventional treatment
process, the coagulation conditions used at each of these plants were
different. These conditions could possibly account for the differences in
NOM removal performance observed among the various WTPs. Finally,
because NOM removal is influenced by the NOM character in raw
water, it is advisable to study the character of NOM to enable the se-
lection of appropriate water treatment processes.
Declaration of conflict of interests
None.
Acknowledgements
This work was funded by the Nanotechnology and Water
Sustainability (NanoWS) Research Unit at the University of South
Africa. We are grateful to all the water treatment plants where sampling
was done; their collaboration is highly appreciated.
Appendix A. Supplementary data
Supplementary material related to this article can be found, in the
online version, at doi:https://doi.org/10.1016/j.jwpe.2019.100809.
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