Chemosphere 309 (2022) 136618

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Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere

Membrane technology as an emergency response against drinking water

shortage in scenarios of dam failure
Roberta N. Guimarães **, Victor R. Moreira *, Míriam C.S. Amaral ***
Department of Sanitation and Environmental Engineering, School of Engineering, Federal University of Minas Gerais, Avenue Antônio Carlos, 6627, Campus Pampulha,
MG, Brazil

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• RO guarantees safe drinking water even

in scenarios of severe water quality
deterioration.
• Fouling was mostly reversible, and the
membranes’ integrity was not compro­
mised after long-term operation.
• UF membrane can retain colloids of As
and Mn, different from sand-filter.
• Variations in feed concentration of As
and Mn do not compromise the RO
permeate quality.
• Provides quantitative/qualitative infor­
mation for treatment decision making.

A R T I C L E I N F O A B S T R A C T

Keywords: With dam failure events, there can be changes in water quality and difficulties in the operation of water treat­
Arsenic ment plants (WTPs) since they were not designed for water treatment under severe pollution conditions. To avoid
Multicriteria analysis that, it was investigated two strategies based on pre-oxidation, ultrafiltration (UF) and reverse osmosis (RO)
Membranes
integrated into a conventional treatment process (coagulation, flocculation, and sand filtration) or with each
Decentralized systems
Centralized systems
other, with the potential to reduce the risks of drinking water shortage and guarantee a safe drinking water
Water treatment supply. The study considered the context of the Velhas river basin (Brazil), where water quality is compromised
by high turbidities (500–3000 NTU) and excessive arsenic (~0.4 mg/L), iron (~50 mg/L), and manganese (~3
mg/L) levels. They were only partially removed by conventional treatments (removals: 74 ± 21%) and potability
standards were only achieved after the membrane separation processes were considered (As: <0.01 mg/L, Mn:
<0.1 mg/L, and Fe: <0.3 mg/L). The high water quality after RO enables its blend with the stream obtained after
sand filters and would allow for greater flexibility during the operation of WTPs operation. Despite the sus­
ceptibility to fouling and most frequent maintenance, the pre-oxidation-UF-RO system would also guarantee a
safe drinking water supply. The decision for the most adequate strategy was then based on a multicriteria
analysis. A retrofit of conventional WTPs by their integration with UF-RO was classified as the best strategy for
centralized facilities, whereas pre-oxidation-UF-RO better fits the reality of decentralized treatments given the
lower costs and deployment time. The methodology based on multicriteria analysis and water treatment

* Corresponding author.
** Corresponding author.
*** Corresponding author.
E-mail addresses: robertanunesg@gmail.com (R.N. Guimarães), victorrznde.eng@gmail.com (V.R. Moreira), miriam@desa.ufmg.br (M.C.S. Amaral).

https://doi.org/10.1016/j.chemosphere.2022.136618
Received 15 July 2022; Received in revised form 12 September 2022; Accepted 25 September 2022
Available online 28 September 2022
0045-6535/© 2022 Elsevier Ltd. All rights reserved.
R.N. Guimarães et al.
technologies, exemplified by membranes in this study, presented satisfactory results for different scenarios of
critical treatment.
1. Introduction
Tailings dams are structures used to store all materials not used after
ore processing. The worldwide number of tailings dams is not yet
conclusive, and the numbers may differ according to the database sur­
veyed. According to the International Commission on Large Dams-
ICOLD, a technical forum on best practices in dam engineering, there
are 57,875 “large” dams in the world that, according to this criteria,
correspond to structures of 15 m or more in height, or, with volumes
greater than 3.000.000 m3 of water (ICOLD, 2021).
Since 1915, a total of 366 incidents were registered worldwide with a
rising trend since 2010. The number might represent only a subset of all
cases and the incidents were mainly located in North American and
European countries (Islam and Murakami, 2021). Most water sources
and sediments were immediately contaminated by tailings after dam
failure, being reported with increased concentrations of dissolved mat­
ter, suspended particulate matter, and trace metals, which persisted
even after six months that the incident was registered (Vergiliodos et al.,
2021). Hatje et al. (2017) reported enrichment factors of 4234 for
mercury in river sediments, 133 of cobalt, 16 of nickel, and other species
that could be remobilized to surface water along with heavy raining
episodes. A commitment to water quality would directly impact human
health given that most impacted water sources are the only drinking
water source for inhabitants located nearby the devasted area. A survey
on trace metals and their concentration in mining tailings (Fig. 1) un­
covers the threat to that these people are subjected. The data presented
reflects contamination resulting from mining tailings from different
extractive activities.
Between 2015 and 2019, in Brazil, two mining tailings dams located
in Minas Gerais collapsed, causing a temporary increase in the concen­
tration of solids and metals resulting from dragging and resuspension.
There was also transport and deposition of natural sediments and tail­
ings materials along the water course channels. The river alluvial sedi­
ments, when subjected to modifying phenomena in a favorable
geochemical environment, are likely to release metals and metalloids
considered harmful to human health, compromising water use. Since
then, the water supply in the regions impacted by the collapsed dams
was made by water tank trucks.
Conventional treatment processes, generally comprised of coagula­
tion, flocculation, and sand filtration was effectively designed to treat
surface water under mild conditions, but are not robust enough to
tolerate harsh conditions (e.g.: elevated turbidity and trace metals
Fig. 1. Trace metals concentration in tailing dams. Adapted from Islam and Murakami (2021).
2
Chemosphere 309 (2022) 136618
concentration) resulting from tailing dams’ failure (Moreira et al.,
2021b).
Considering that, membrane separation processes could act as rein­
forcement to conventional treatments or be employed as decentralized
units (Hoslett et al., 2018; Moreira et al., 2022). These processes
generally have low area requirements, reduced time for deployment,
and are commercialized as mobile units, characteristics that favor their
use in emergencies.
Ultrafiltration (UF) membranes could considerably improve the
drinking water quality and can retain most microorganisms and sus­
pended matter (Yu et al., 2020). When integrated into conventional
treatment processes, UF acts as an additional barrier to colloids and
precipitated formed, including those containing arsenic and manganese
(Moreira et al., 2021c). However, complexes of arsenic and manganese
do not often occur and these species, along with other trace metals in
tailings composition, are commonly found in their dissolved form with
low expectations to be removed by UF membranes.
One alternative would be the conversion of dissolved species into
their colloidal forms by pre-oxidation processes. Although effective,
these are processes still subjected to the surface water quality that could
have in its composition other compounds that are preferably oxidized
over trace metals. That justifies the use of more restrictive membranes as
reverse osmosis (RO), capable to retain even the dissolved species of
monovalent ions (Ritt et al., 2022). Despite the greater efficiency in the
removal of organic, inorganic, or biological pollutants (Albergamo et al.,
2019; Chen et al., 2020; Sousi et al., 2020), RO has also a greater energy
demand compared to UF membranes and is more susceptible to fouling,
two aspects that should limit its application to centralized drinking
water treatment plants. Advancements in membranes of greater
permeability and lower susceptibility to fouling did occur in recent
years, but most developments remained as scientific reports and only 8%
were commercialized (Ritt et al., 2022).
A previous review paper presented by Guimarães et al. (2022)
focused on the impact on water quality after rupture events and the
necessity for water treatment plants to improve their processes to
guarantee a safe drinking water supply. Unfortunately, the legislative
framework is deficient in this aspect, and so it is the studies that
investigated the performance of water treatment plants under harsh
conditions that surface water encountered after these accidents.
To guarantee a safe drinking water supply, this study investigates
pre-oxidation, UF, and RO strategies to enhance drinking water treat­
ment performance in emergencies such as tailing dams collapse. These
R.N. Guimarães et al. Chemosphere 309 (2022) 136618

are consolidated technologies, but their integration with conventional and then compared with systems integrated into UF and RO membranes
treatment processes for a safe drinking water supply was not assessed as reinforcements. Pre-oxidation-UF-RO, all integrated, were also eval­
yet. A conventional treatment process comprised of pre-oxidation, uated for their potential for water treatment. In the end, a multicriteria
coagulation-flocculation, and sand filtration was initially evaluated analysis is proposed to assist the decision for the most adequate strategy

Fig. 2. Map of tailings dams in the Velhas River basin.

3
R.N. Guimarães et al.
considering the following variables: performance/robustness, level of
control, waste generation, implementation area, deployment time, and
cost.
2. Materials and methods
2.1. Study area description
The Velhas river basin is in the central region of Minas Gerais
(Brazil), between latitudes 17◦ 15′ S and 20◦ 25′ S and longitudes 43◦ 25′ W
and 44◦ 50′ W. The basin comprises an area of 27,850 km2. The region
referred to as Alto Velhas (located in the Velhas river basins; Fig. 2)
comprises ten municipalities and has the largest population contingent,
with significant economic activity. In this region, the main polluting
agents are untreated industrial and domestic wastewater. The Alto
Velhas has also the largest contingent of mining tailings dams (10% of
tailing dams installed in Brazil). That could represent a potential risk in
terms of water supply in scenarios of tailings dams’ rupture. Upstream
the Drinking Water Treatment Plant of Bela Fama (facility also repre­
sented in Fig. 2) is installed several 50 tailing damns, most of them
responsible to store mining tailings as shown in Fig. 3. The Drinking
Water Treatment Plant attains the necessity of approximately 2.1
million people in nine municipalities.
Previous analysis of the river sediments collected in the basins, close
to the water treatment plant mentioned, pointed to a high iron con­
centration, approximately 2–4 times greater than the average content of
the Earth’s crust (4.2%), with an order of magnitude similar to those
found in mining tailings. Conversely, river sediments and mining tail­
ings are aluminum-depleted, which suggests a clay-depleted material
(alumino-silicates). The manganese contents in the sediments and tail­
ings are close to or within the average values referring to the Earth’s
crust (0.1%).
Among all the elements assessed, the high arsenic concentrations
represented a major point of concern. All the samples studied present
arsenic levels above 5.9 mg/kg, and 50% of the samples collected exceed
values of 17.0 mg/kg (minimum: 8.1 mg/kg; maximum: 29.2 mg/kg).
The element concentration is higher in river sediments compared to
mining tailings. Other compounds such as chromium, nickel, and cop­
per, although assessed, were present in smaller proportions.
The atypical characteristics of river sediments in terms of iron,
manganese, and arsenic would already justify studies for water treat­
ment plant reinforcements. Depending on modifying phenomena and
the geochemical environment, the species mentioned tend to resolu­
bilize, compromising water use. After all, based on the basin’s impor­
tance for water supply, aligned with the remarkable presence of tailing
damns and hydrogeochemical characteristics, motivated an in-depth
study of the basin in a hypothetical scenario of dam failure.
2.2. Sample collection and analysis
Surface water used in this study was collected in the Alto Velhas
region. Based on the latest monitoring report made available by envi­
ronmental agencies, the arsenic concentration values varied from 0.015
to 0.4 mg/L (spiked with: Na2HAsO4⋅7H2O; CAS: 10,048-95-0), 0.13–50
mg/L for iron (spiked with: FeCl3; CAS: 7705-08-0), and 0.48–1.5 mg/L
for manganese (spiked with: MnSO4⋅H2O; CAS: 10,034-96-5) (IGAMdas
Á, 2019). These concentration values were defined as spiking limits in
the current study. Once collected, the water samples were stored in the
absence of light at temperatures below 4 ◦ C and brought to room tem­
perature before their use and characterization. The surface water was
characterized in terms of its physicochemical properties, according to
the Standard Methods for The Examination of Water and Wastewater.
Instruments used to measure turbidity, electrical conductivity, pH,
redox potential, and color were, Hach 2100Q, MS Tecnopon mCA-150,
MS Tecnopon mPA-210, Hach HQ11D, and Hach DR3900. Iron, man­
ganese, and arsenic concentration values were determined by
4
Chemosphere 309 (2022) 136618
inductively coupled plasma mass spectrometry (Agilent ICP-MS 7700;
method 3125B). Dissolved and colloidal fractions of these species were
estimated using siring filters (0.45 μm; 0.22 μm and 0.04 μm). Fractions
retained by 0.45–0.22 μm filters were classified as colloidal whereas
fractions retained by 0.04 μm filters were classified as dissolved.
2.3. Experimental design
Experimental conditions were summarized in Fig. 3 and Table S1
(supplementary material). It was tested how different turbidities and
concentrations of arsenic, iron, and manganese impacted the efficiency
of conventional treatment processes and the retention efficiency of UF
and RO membranes. The experiments used a hollow fiber submerged UF
module and a spiral-wound RO module, in both cases coupled to a
manometer, pump, and a rotameter to measure the permeate flow rate.
The membranes were physically cleaned by recirculating deionized
water, followed by a backwashing procedure for 5 min. In case the
membrane’s permeability was not restored, a chemical cleaning pro­
cedure was made and consisted of an ultrasonic bath with NaOH (0.2 wt
%) and citric acid (pH = 2.5) for 20 min each.
Two different scenarios were considered and represented in Fig. 3.
The first one would be the retrofit of conventional drinking water
treatment plants by their integration to pre-oxidation and advanced
treatments based on UF and RO. That could represent the reality of
centralized treatment plants already under operation. Alternatively,
integrated pre-oxidation and membrane separation processes (UF-RO,
also represented in Fig. 3) could be an option for decentralized treat­
ments. The modularity and short deployment time associated with these
systems would allow their use under an emergency scenario of mining
tailing dams’ rupture.
Permeate flux (J) was calculated by Equation (1), in which Δv is the
permeate volume (L) collected at a given time interval Δt (h) and sm is
the effective membrane area (m2). The fouling propensity was evaluated
by the membrane pore blocking models developed by Hermia (1982).
( )
J
L
=
Δv
(1)
m2 h sm × Δt
The total resistance to filtration (Rt , Equation (2)) was also moni­
tored. In Equation (2), k (m3/m2.s.Pa) represents the membrane
permeability during the filtration experiments with groundwater and
μ(25◦ C) the dynamic viscosity of water at 25 ◦ C (8.9 × 10− 4 Pa s).
Assuming that the membrane resistance would not change, the increase
in Rt would be mainly associated with fouling formation onto the
membrane surface.
( )
1 1
Rt = (2)
m k.μ(25◦ C)
2.4. Multi-criteria decision analysis (MCDA)
The most appropriate strategy of water treatment for each scenario
was defined based on multi-criteria decision analysis (MCDA) and the
weighted summation method. The utility of each alternative (uj ) was
estimated by summing up the weighted (wi ) numerical values of each
criterion (sij , ), Equation 3. The strategy presenting the greatest utility
(uopt ), Equation (4) was defined as the best alternative under the sce­
nario and criteria considered. That should represent advancements from
past studies that considered a single criterion approach based solely on
capital and operational costs (Victor Rezende Moreira et al., 2021b;
2021a) since it would account for various dimensions while deciding on
the most appropriate strategy.
∑
m
uj = wi sij , for all j (3)
i=1
R.N. Guimarães et al.
Fig. 3. Representations of the integrated systems along with their experimental conditions.
( )
uopt = max uj , for all j (4)
Six different criteria were defined based on a top-down approach
(Keeney and McDaniels, 1992) and considering the primary goal of a
safe drinking water supply in cases of water contamination by mining
tailings. The criteria were summarized in Table 1 and included (i) per­
formance and robustness; (ii) level of control; (iii) waste generation; (iv)
deployment area; (v) deployment time; and (vi) costs. All six criteria
were ranked from 1 to 5, in which 1 was defined as very weak (worst
performance according to the criterion), 2 as weak, 3 as average, 4 as
strong, and 5 as very strong (best performance according to the
criterion).
2.5. Statistical analysis
Microsoft Excel and OriginPro were used for statistical and data
analysis. Although the results had a trend for a normal distribution,
verified by the Shapiro-Wilk’s test and Levene’s test for homogeneity,
Mann-Whitney U Test and Spearman were preferred for comparison
between two independent groups and correlation. Mann-Kendall trend
tests were made to verify a possible trend for flux decay. A confidence
level of 95% was set for all statistical analyses performed.
3. Results and discussions
3.1. Conventional treatment and its performance for arsenic, iron, and
manganese removal
Excessive levels of arsenic, iron, and manganese would be the main
factors compromising water quality. For that reason, the residual con­
centration of all three species was monitored after each treatment unit
(Table 2). Pre-oxidation and floc formation by colloidal particle desta­
bilization during coagulation could favor the obtainment of amorphous
species of ferric hydroxide. These could entrap dissolved species of
arsenic, iron, and manganese, being removed in the settling tanks. If not,
the remaining suspended fractions could be retained by sand filters.
Different from suspended fractions, the dissolved species of arsenic,
iron, and manganese would pass through the treatment process without
being removed. Depending on the surface water characteristic, the dis­
solved fraction of arsenic and manganese could represent up to 38% and
5
Chemosphere 309 (2022) 136618
59%, respectively, of their total concentration (Fig. 4). That would also
explain the concentration of arsenic and manganese above the threshold
values for drinking water after sand filters (arsenic: 0.01 mg/L and
manganese: 0.1 mg/L). The manganese ions are thermodynamically
more stable in their reduced and soluble form (Mn2+) being more
difficult to be oxidized to Mn3+ and Mn4+ and later removed as a
complex. When oxidation occurs, the size of the complexes formed
(mainly manganese dioxide) is in a sub-colloidal size range and of low
settling rate and is not removed after settling tanks nor retained by sand
filters (Tobiason et al., 2016).
Complementary, positive correlations were found between residual
turbidity and residual concentrations of arsenic and manganese (rSpear­
man = 0.771; rSpearman = 0.948). That also explains the concentrations
above the recommended values for both species given that suspended
particles responsible for medium turbidity could act as a carrier to dis­
solved fractions that were not oxidized (Victor Rezende Moreira et al.,
2021b). For these conditions, the oxidation step becomes more impor­
tant, and larger oxidant doses would be required. It is important to
mention that in the event of a dam failure, a high concentration of solids
is expected to occur and this high concentration will bring challenges to
the water treatment plant operation. For instance, it is possible to
mention that stricter chemical control would be required to ensure
arsenic and manganese removal, which becomes even more challenging.
Another alternative would be a reinforcement in the solid/liquid
separation step, employing processes with greater effectiveness in the
removal of sub-colloidal particles. They would act not only in the
removal of dissolved species of arsenic and manganese but also in the
remained suspended particles responsible for medium turbidity.
3.2. UF and RO as tertiary treatments
The variability of the streams obtained after the sand filter was not
enough to compromise the UF permeate flux (58.7 ± 6.8 L/m2h) and the
differences observed were considered non-significant (p = 0.059)
(Table 3). The efficiency of UF assessed under different initial conditions
demonstrated that the threshold values for arsenic, iron, and manganese
were achieved in all cases. Like sand filters, UF would not act on dis­
solved fractions but would remove the remaining turbidity acting as a
carrier. In a hypothetical scenario of dam failure in the Velhas basin, UF
R.N. Guimarães et al. Chemosphere 309 (2022) 136618

Table 1 but the differences in the remaining concentration values of the dis­
Criteria and evaluation methods considered in the multi-criteria analysis. solved species were considered non-significant for all three contami­
Criteria Description Classification Evaluation mode nants and within the recommended values. The process would also
withstand possible variations in arsenic and manganese concentrations
1. Performance Likelihood to Higher the Qualitative
and withstand abnormal best assessment from as observed after sand filters and would represent a secure alternative to
robustness operation conditions technical data guarantee drinking water standards in cases of lower efficiency of con­
and operation safety available for each ventional treatment processes. Greater efficiency is expected for RO
margins concerning system and scenario ( membranes, that reject contaminants based on their size and charge. Its
the treatment Victor Rezende
objectives Moreira et al., 2021b;
integration with UF complies with multi-barrier approaches, an
2021a), including approach considered as the most effective way to manage drinking
data from the current water systems aiming to reduce the risk of drinking water contamination
study (Yu et al., 2018).
2. Level of High automation and Lower the Subjective qualitative
The efficiency of RO was further assessed for different arsenic con­
control the need for skilled best assessment from past
labor to operate experiences for each centrations (iron and manganese concentrations were kept constant)
automated systems system and scenario considering that the element would represent the greatest risk to human
3. Waste Waste is generated Lower the Subjective qualitative health among all species (Fig. 5). The concentration values were defined
generation during treatment best assessment from past based on the removal efficiency of coagulation-flocculation and sand
processes (e.g.: experiences and
residual sludge) or technical data
filtration processes, and considering that arsenic would be predomi­
after the end of available for each nantly dissolved and not removed by UF membranes. The long-term
equipment’s working system and scenario monitoring data demonstrated to have a Kendall correlation for flux
life (e.g.: end-of-life (Cremades et al., decay (p < 0.001) over the operation time, corresponding to 14%. Apart
membranes). 2018; Lawler et al.,
from that, the system was able to attain the drinking water standards for
2015)
4. Deployment Area required to Lower the Subjective qualitative all three species. Despite the flux decay, the permeability values before
area install new systems or best assessment from past the tests and after membrane cleaning were 3.47 and 3.82 L/m2.h.bar.
upgrade existing ones experiences and The similarity suggests that the cleaning procedures were effective in
in a hypothetical technical data fouling removal, in that case, considered mostly reversible, and that the
scenario of dam available for each
membrane integrity was not compromised. The residual concentration
failure and water system and scenario
quality commitment (Hofs et al., 2022) values of arsenic, iron and manganese had no monotonic trend, attested
5. Deployment Time required to Lower the Subjective qualitative by Kendall correlation tests (p < 0.001), and the variability observed is
time install new systems or best evaluation from past most probably associated with random events.
upgrade existing ones experiences (Hofs
The high water quality after RO enables its blend with the stream
in a hypothetical et al., 2022)
scenario of dam obtained after sand filters and would confer to the drinking water
failure and water treatment plant greater flexibility during its operation. That would
quality commitment reduce the total water volume treated by the membrane units without
6. Costs Impacts of Lower the Assessment from compromising the plant capacity in water supply and would lower the
deployment and best quotations and real
treated water corrosivity once desalinated by RO (Lesimple et al., 2020).
operational costs for costs of similar
each scenario where treatment facilities ( Table 4 demonstrates the blend ratio required to guarantee that the
the system will be Victor Rezende maximum level of arsenic in drinking water would still be attained. As
installed and costs for Moreira et al., 2021b; the arsenic concentration leaving the sand filters increases, so increases
potential system 2021a)
the RO permeate requirement and the arsenic concentration in RO
upgrading
concentrate.
Proper management of the concentrate stream produced should be
could also act on the colloidal and subcolloidal (size: > 0.20 μm) frac­ then considered. The UF concentrate could be recycled back to the inlet
tions of aluminum, nickel, copper, and chromium, expected to be pre­ of the drinking water treatment plant. The UF concentrate would
sent (Silva et al., 2022). represent minor contributions to the surface water quality in an eventual
Conversely, most dissolved ionic species in the medium would scenario of dam rupture. In this sense, there are low expectations that
remain, especially those from arsenic, iron, and manganese which have the treatment efficiency would be compromised. The hypothesis was
hydrated radii in the order of nanometers or smaller (Marcus, 1988) and investigated, and the results are reported in Table 5. The data suggest
would not be retained by steric hindrance. Therefore, greater robustness that the physicochemical characteristics along the treatment trail tend to
would be achieved when the UF permeate is further treated by RO. reduce at successive recirculation processes. In that sense, the UF
The process would have a lower permeate flux (25.1 ± 1.5 L/m2h), concentrate recirculation would dilute the feed stream entering the

Table 2
Characterization of turbidity, arsenic (As), iron (Fe), and manganese (Mn) at different treatment stages of conventional treatment processes. *WS stands for “water
sample”.
Initial conditions After settling tanks After sand filters

Turbidity Concentration of arsenic (As), iron (Fe), Turbidity As (mg/L) Fe (mg/ Mn (mg/ Turbidity As (mg/L) Fe (mg/ Mn (mg/
(NTU) and manganese (Mn) (NTU) L) ) (NTU) L) L)

1000 WS1 – As: 0.015 mg/L; Fe: 0.13 mg/L; Mn: 1.64 ± 0.22 0.009 ± 0.13 ± 0.38 ± 0.41 ± 0.04 0.007 ± 0.07 ± 0.22 ±
0.48 mg/L 0.001 0.01 0.06 0.004 0.01 0.01
WS2 – As: 0.1 mg/L; Fe: 12.5 mg/L; Mn: 1.86 ± 0.27 0.013 ± 0.62 ± 0.45 ± 0.29 ± 0.02 0.010 ± 0.10 ± 0.34 ±
0.75 mg/L 0.003 0.09 0.02 0.002 0.02 0.02
WS3 – As: 0.2 mg/L; Fe: 25 mg/L; Mn: 1.5 1.36 ± 0.26 0.010 ± 0.30 ± 1.08 ± 0.40 ± 0.06 0.007 ± 0.11 ± 0.48 ±
mg/L 0.002 0.02 0.09 0.002 0.02 0.06
WS4 – As: 0.4 mg/L; Fe: 50 mg/L; Mn: 3 1.46 ± 0.41 0.022 ± 0.23 ± 2.28 ± 0.41 ± 0.03 0.014 ± 0.10 ± 1.72 ±
mg/L 0.003 0.06 0.01 0.004 0.02 0.01

6
R.N. Guimarães et al. Chemosphere 309 (2022) 136618

Fig. 4. Dissolved and colloidal fractions of arsenic, iron, and manganese remaining after sand filters. Initial conditions WS1 – As: 0.015 mg/L; Fe: 0.13 mg/L; Mn:
0.48 mg/L; WS2 – As: 0.1 mg/L; Fe: 12.5 mg/L; Mn: 0.75 mg/L; WS3 – As: 0.2 mg/L; Fe: 25 mg/L; Mn: 1.5 mg/L; and WS4 – As: 0.4 mg/L; Fe: 50 mg/L; Mn: 3 mg/L.

Table 3
Permeate flux and residual concentrations of arsenic, iron, and manganese for UF and RO. WS1: 0.015 mg/L of As, 0.13 mg/L of Fe, and 0.48 mg/L of Mn; WS2: 0.1 mg/
L of As, 0.75 mg/L of Fe, and 0.75 mg/L of Mn; WS3: 0.2 mg/L of As, 25 mg/L of Fe, and 1.5 mg/L of Mn; and WS4: 0.4 mg/L of As, 50 mg/L of Fe, and 3 mg/L of Mn, all
at initial turbidity of 1000 NTU.
Ultrafiltration Reverse osmosis

Permeate flux (L/m2h) Arsenic (mg/L) Iron (mg/L) Manganese (mg/l) Permeate flux (L/m2h) Arsenic (mg/L) Iron (mg/L) Manganese (mg/L)

WS1 53.0 ± 1.1 0.003 ± 0.001 0.07 ± 0.02 0.131 ± 0.018 24.2 ± 2.4 0.001 ± 0.001 0.02 ± 0.01 0.019 ± 0.003
WS2 63.9 ± 2.0 0.002 ± 0.001 0.06 ± 0.02 0.098 ± 0.004 27.1 ± 1.2 0.001 ± 0.001 0.03 ± 0.01 0.021 ± 0.003
WS3 65.4 ± 1.7 0.006 ± 0.002 0.08 ± 0.01 0.166 ± 0.021 25.5 ± 0.7 0.001 ± 0.001 0.03 ± 0.01 0.020 ± 0.002
WS4 52.8 ± 1.1 0.004 ± 0.001 0.08 ± 0.01 0.590 ± 0.009 23.8 ± 0.9 0.001 ± 0.001 0.02 ± 0.01 0.020 ± 0.003

Table 4
Blend ratio for a maximum level of arsenic in drinking water within recom­
mended values (10 μg/L). Qsf: sand filter outlet flowrate, Qp: RO permeate
flowrate, Qc: RO concentrate flowrate. Values were estimated by mass balance
considering the sand filter outlet and the RO system as a control volume. The
concentrations of iron (0.05 mg/L) and manages (0.039 mg/L) were kept con­
stant in this experiment.
Arsenic (mg/L) Qsf Ratio RO concentrate characteristics
(m3/s) Qp/Qsf
After sand RO Qc As Mn
filtration permeate (m3/s) (mg/L) (mg/L)

0.013 0.001 9 25% 0.529 0.064 0.817

0.020 53% 1.046 0.099
0.015 36% 0.737 0.074
0.018 47% 0.953 0.089
0.030 77% 1.451 0.148
0.040 69% 1.323 0.198

3.3. Integrated pre-oxidation, UF, and RO

Fig. 5. Reverse osmosis monitoring treating water samples at different arsenic
concentrations. The concentrations of iron (0.05 mg/L) and manages (0.039
mg/L) were kept constant in this experiment.
treatment processes rather than increase its complexity. Another
advantage would be the lower adduction flow rate required to attain the
same flow rate of treated water.
The RO concentrate also presented mild conditions and its physico­
chemical characterization was within the threshold values for discharge
in receiving bodies (Table S2, supplementary material). The values ob­
tained were not high enough to justify the use of evaporation and
crystallization techniques as employed for brine solutions obtained from
desalination plants (Subramani and Jacangelo, 2014). Complementary
studies that investigate the environmental impact of concentrate
disposal in surface water could complement the alternative mentioned.
Up to date, most studies focused on environmental impacts associated
with brines’ disposal (Valdés et al., 2021), which differ in composition
from the concentrate obtained from RO system employed as advanced
treatment in surface water treatment plants.
Results for UF and RO integrated and preceded by pre-oxidation
processes were summarized in Fig. 6. It is noticed that UF has a sharp
flux decline at the beginning of the operation, most probably due to
concentration polarization effects, and stabilized after 180 min opera­
tion. That corresponded to a 31% of flux decline (J0: 147.6 and Jf: 101.5
L/m2h). Fouling resulted from a cake layer formation (r2 = 0.914; ks =
8.55 10− 4 1/s) composed of suspended matter, colloids, and precipitates
that would have formed after pre-oxidation processes. Nevertheless, the
cake layer was easily removed after the physical cleaning, not being
required the use of chemicals or additives to restore the membrane
permeability.
It is noticed variability in residual concentrations of iron, arsenic,
and manganese in UF permeate, the two latter above their maximum
contaminant levels. That justified the integration of an additional pol­
ishing process as RO. Its rejection capacity guaranteed the drinking
water quality, however with higher energy demand and lower permeate
flux. Its average permeate flux corresponded to 18.1 ± 0.4 L/m2h, with a
lower flux decay (<5%) compared with UF. The results emphasize the
advantages of an integrated system, in which UF served well as pre-

7
R.N. Guimarães et al. Chemosphere 309 (2022) 136618

Table 5
Ultrafiltration (UF) concentrate recirculation to feed stream and its impact on removal efficiencies of sand filters, ultrafiltration, and reverse osmosis.
Concentrate recirculation loop Parameters Feed water Sand filters UF permeate UF concentrate RO permeate RO concentrate

1 Turbidity (NTU) 1068 ± 8 0.41 ± 0.01 0.26 ± 0.01 5.61 ± 0.03 0.07 ± 0.01 0.59 ± 0.04
Arsenic (mg/L) 0.200 ± 0.010 0.011 ± 0.006 0.007 ± 0.001 – <0.001 0.013 ± 0.002
Iron (mg/L) 25 ± 0.30 0.13 ± 0.01 0.04 ± 0.01 – 0.06 ± 0.01 0.15 ± 0.01
Manganese (mg/L) 1.500 ± 0.100 0.039 ± 0.001 0.026 ± 0.001 – 0.013 ± 0.001 0.122 ± 0.003
2 Turbidity (NTU) 993 ± 38 0.45 ± 0.12 0.09 ± 0.01 3.56 ± 0.09 0.07 ± 0.01 0.33 ± 0.01
Arsenic (mg/L) 0.198 ± 0.019 0.010 ± 0.010 0.006 ± 0.002 – <0.001 0.011 ± 0.002
Iron (mg/L) 23.17 ± 0.12 0.12 ± 0.01 0.02 ± 0.01 – 0.04 ± 0.01 0.08 ± 0.01
Manganese (mg/L) 1.430 ± 0.001 0.041 ± 0.001 0.028 ± 0.001 – 0.016 ± 0.010 0.120 ± 0.001
3 Turbidity (NTU) 971 ± 13 0.41 ± 0.03 0.17 ± 0.01 6.10 ± 0.69 0.07 ± 0.01 0.24 ± 0.002
Arsenic (mg/L) 0.191 ± 0.001 0.010 ± 0.001 0.009 ± 0.001 – <0.001 0.010 ± 0.002
Iron (mg/L) 24.13 ± 0.12 0.13 ± 0.01 0.04 ± 0.01 – 0.03 ± 0.01 0.07 ± 0.01
Manganese (mg/L) 1.205 ± 0.001 0.034 ± 0.001 0.029 ± 0.001 – 0.013 ± 0.001 0.065 ± 0.03
4 Turbidity (NTU) 982 ± 7 0.41 ± 0.01 0.09 ± 0.01 5.04 ± 0.91 0.06 ± 0.01 0.51 ± 0.06
Arsenic (mg/L) 0.181 ± 0.001 0.011 ± 0.001 0.007 ± 0.002 – <0.001 0.012 ± 0.001
Iron (mg/L) 22.73 ± 0.12 0.14 ± 0.01 0.03 ± 0.01 – 0.03 ± 0.01 0.08 ± 0.03
Manganese (mg/L) 1.405 ± 0.001 0.034 ± 0.001 0.030 ± 0.001 – 0.013 ± 0.001 0.121 ± 0.010

Fig. 6. Monitoring data for UF and RO preceded by the pre-oxidation process. As, Fe, Mn (mg/L) refers to residual concentration values in the permeate. Initial water
turbidity: 1000 NTU.

treatment to RO, membranes that would be more susceptible to fouling.
RO, in turn, demonstrated to be a robust technology to treat contami­
nated water under the harsh conditions considered. Similar observations
were possible when the permeate turbidity was compared, for UF its
average value corresponded to 0.16 ± 0.04 NTU, and for RO 0.04 ± 0.02
NTU. The high quality of RO permeate might still allow for its blend with
UF permeate. That would reduce the requirements of RO systems (e.g.:
membrane area and energy) without compromising the safety of the
water being supplied.
The differences in rejection efficiency of UF and RO could be
explained by their morphology. UF is a porous membrane with an
average pore size of 0,1 μm, sometimes greater than the complexes of
iron, arsenic, and manganese formed (Victor Rezende Moreira et al.,
2021a). For being porous, UF imposes a lower resistance to filtration and
yields a higher permeate flux, but it has lower rejection efficiency. RO,
in turn, is no longer defined by its pores and is recognized for being a
dense membrane. The transport mechanisms across RO membranes are
driven by diffusion principles (Greenlee et al., 2009), which explains its
greater efficiency but lower permeate flux.
The integrated processes of pre-oxidation, UF, and RO were efficient
in water treatment but compared with conventional treatment processes
followed by UF and RO, it most probably would require high membrane
maintenance (e.g.: cleaning frequency, which reduced membrane life­
span and would imply in more frequent membrane replacement) given
the higher flux decay. That could represent a higher level of control,
which should be considered along with their performance, waste gen­
eration, implementation area, deployment time, and costs in multi­
criteria analysis.
3.4. Comparison between the integrated processes by MCDA
Two scenarios were considered, centralized (population equivalent:

8
R.N. Guimarães et al. Chemosphere 309 (2022) 136618

≥ 50,000 (Obermann and Sattler, 2013)) and decentralized treatments of energy failure, most water treatment plants have an emergency en­
(population equivalent: ≤ 10,000 (Obermann and Sattler, 2013)), ergy supply, whereas decentralized units would interrupt their opera­
against both strategies presented, conventional treatment processes in­ tion (Vieira et al., 2008).
tegrated to pre-oxidation-UF-RO (strategy 1) and integrated processes of Wastes production and management deserve special attention. While
pre-oxidation-UF-RO (strategy 2). The performance matrix is presented the disposal of end-of-life membranes is a factor in common in both
in Table 6. strategies, strategy 1 accounted with conventional treatment processes
Compliance with drinking water standards became a point of still needs to properly manage the exhausted waste, process water pro­
concern for drinking water treatment plants comprised of coagulation- duced, and mainly the sludge produced in the settling units, especially
flocculation and sand filtration, starting at the plant outlet and aggra­ under high turbidity conditions.
vated at the consumption point. When operated under mild surface Environmental management tools such as life cycle assessment (LCA)
water conditions, the processes employed could be satisfactory in enable the assessment of potential environmental consequences derived
pollutant removal. The issues start to be observed under harsh condi­ from end-of-life membranes. Lawler et al. (2015) compared seven
tions, whether high turbidity and trace metals concentration as evalu­ different alternatives for the disposal of membrane elements, being
ated or the presence of other pollutants resulting from anthropogenic incineration and landfill disposal the options with the most impact on
activities. The average removal of micropollutants, for example, tends to climate change. Membrane reuse (e.g.: by recycling procedures) would
be significantly lower for conventional treatment plants (~38%) be the most environmentally favorable. Apart from proper membrane
compared with those plants that employ advanced treatments and other disposal, strategy 1 still needs to consider the sludge derived from its
filtration processes (~60–65%) (Tröger et al., 2020). Despite that, process. The challenge in its disposal is due to the presence of trace
conventional processes still act as a barrier to these pollutants that, metals and other pollutants removed from raw water, besides the
although not effective, could be a better scenario compared to remote chemicals used during pre-oxidation, coagulation, and flocculation
regions that deal with the burdens of drinking water accessibility and processes. Until the end of the 20th century, most sludges were directly
the lack of treatment systems (Byrne et al., 2021; Komatsu et al., 2020). discharged into surface water or by deep wells injection, a practice
That suggests that decentralized treatments would require a higher prohibited nowadays in some developed countries (Cremades et al.,
level of robustness compared with centralized treatments that already 2018). The high transportation costs and strict regulatory guidelines
have additional processes to alleviate the harsh conditions that surface make its incorporation in agricultural soils a prohibitive practice,
water may be encountered. A recent survey of isolated regions revealed especially due to the presence of trace metals, and sludge is also a poor
that Escherichia coli was detected in all sampled sources, including wells, candidate for incineration due to its low organic content and calorific
springs, and rainwater tanks suggesting fecal matter contamination in value (Cremades et al., 2018). For these reasons, sludges from drinking
water sources intended for consumption (Byrne et al., 2021). Regardless water treatment plants are often disposed of in sanitary landfills.
of the scenario, access to a safe drinking water supply by effective sys­ Deployment area, time, and costs are closely related to the treatment
tems prevents several human health issues and is an aspect that deserves scale. Small water systems are in principle more versatile and could be
special attention (Ashbolt, 2015). an option for centralized and decentralized systems given their lower
By level of control, it is considered mainly online water quality deployment area, time, and costs. These are characteristics of the units
monitoring, an important aspect in both centralized and decentralized of UF-RO considered in strategy 2, which could be preassembled in a
units and regardless of the strategy. Conventional treatment processes factory, skid-mounted, transported to the site, and be virtually operated.
should better deal with the deployment of additional monitoring sys­ On the contrary, processes comprised of conventional treatments
tems as they commonly account for automatic systems for chemical generally have high implementation, maintenance, and operating costs
dosages and sludge discharges, besides online water quality monitoring since they have significant infrastructure (treatment units, reservoirs,
that already exists in these facilities. Although important for decen­ and water distribution main), automated monitors, control systems, and
tralized units, most isolated regions have limited access to grid con­ on-site operators. A recent comparison was made between conventional
nections to secure the energy required by these systems. That treatment processes and UF employed for drinking water obtainment
emphasizes the importance of robust treatments in these cases. In events and reinforced the high expenditures of conventional processes (US$
0.73–0.90/m3, compared with 0.07–0.08 US$/m3 for UF) (Moreira
Table 6 et al., 2021b).
Alternatives and their scores against the criteria in a performance matrix. In an eventual scenario of dams-rupture, the faster deployment time
Strategy 1 corresponded to the integration of pre-oxidation, UF, and RO in a and low area requirement of strategy 2 could come in handy with the
conventional drinking water treatment, and Strategy 2 corresponded to the in­ necessity for drinking water supply either in centralized or decentralized
tegrated process of pre-oxidation-UF-RO. scenarios. That is a complex scenario, though, and should be evaluated
Criteria and objectives sij Scenario 1: Scenario 2: with caution. Other pollutants washed down along the rupture such as
Centralized treatment Decentralized mainly undissolved trash could require additional units for their
of drinking water – treatment of drinking removal. Deployment area becomes an important factor especially in
Weights (wi ) water – Weights (wi )
cases of centralized systems, generally located in or near urbanized areas
Strategy Strategy Strategy Strategy with low availability of installation area.
1 2 1 2
Based on the overview given, utility and weight values were assigned
1. Maximization of 5 0.30 0.24 0.27 0.24 to each criterion considering the different scenarios and strategies,
performance/ based on the researchers’ expertise and literature studies that considered
robustness
2. Minimization of Level 2 0.17 0.11 0.08 0.06
MCDA as a decision tool for drinking water treatment systems (Sudha­
of control required karan et al., 2013). The strategy presenting the greatest utility was then
3. Minimization of waste 4 0.10 0.14 0.07 0.16 defined as the best alternative under the scenario and criteria consid­
generation ered. Strategy 1 and 2 are quite comparable when centralized units are
4. Minimization of 3 0.11 0.12 0.17 0.21
considered, especially because most of them are already had coagula­
deployment area
required tion, flocculation, and sand filters. In both strategies, the implementa­
5. Minimization of 5 0.13 0.15 0.11 0.14 tion would be mainly associated with the membrane filtration units.
deployment time That is not the case for decentralized treatments, in which the best
6. Costs 5 0.19 0.21 0.09 0.19 alternative after MCDA analysis was proven to be the second strategy
∑m
i=1 wi sij
– 4.17 4.14 3.30 4.24
(pre-oxidation-UF-RO) mainly because of the lower costs and

9
R.N. Guimarães et al.
deployment time.
4. Final considerations
The recurrence of environmental disasters and the consequent
compromise of surface water quality demands proper strategies from
centralized and decentralized water treatment to ensure a safe drinking
water supply. The contribution of UF and RO became evident after being
demonstrated that the conventional processes of coagulation, floccula­
tion, and sand filtration failed in attaining the threshold values of
arsenic (>0.01 mg/L) and manganese (>0.1 mg/L) for drinking water.
On contrary, potability standards were achieved for RO permeate even
under harsh conditions that surface water is encountered after mining
tailing damns rupture. The average permeate flux for RO was 18.1 L/m2.
h, a process that performs within expectance and with low flux-decay at
long-term operations (J/J0 > 0.85). A retrofit of conventional drinking
water treatment plants by their integration with UF-RO was classified as
the best strategy for centralized facilities. That is not the case for
decentralized treatments, in which the best alternative defined after a
multicriteria analysis was proven to be the implementation of a pre-
oxidation-UF-RO mainly because of the lower costs and deployment
time. In summary, the findings presented in this study may further
support emergency plans in unexpected scenarios of water deterioration
as encountered after tailing dam failures. The outcomes covered aspects
of water treatment under harsh conditions not previously found in
current literature, being an important step to guarantee a safe drinking
water supply by centralized and decentralized drinking water treatment
plants.
Credit author statement
Roberta N. Guimarães: Conceptualization, Formal analysis, Visuali­
zation, Writing – original draft, Writing – review & editing. Victor R.
Moreira: Conceptualization, Formal analysis, Visualization, Writing –
original draft, Writing – review & editing. Míriam Cristina Santos
Amaral: Conceptualization, Formal analysis, Visualization, Writing –
original draft, Writing – review & editing, Resources, Supervision.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgments
The authors acknowledge the kind support provided by the Com­
panhia Vale do Rio Doce (Vale S.A.) for data provision, and the Coor­
dination of Superior Level Staff Improvement (CAPES), the National
Council for Scientific and Technological Development (CNPq), and the
Foundation for Research Support of the State of Minas Gerais (FAPE­
MIG) for financial resources.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.chemosphere.2022.136618.
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