Copper Removal from Industrial Wastewater: A Comprehensive Review

Abstract

Copper is one of the most valuable and prevalent metals used in the industry. There are many techniques to treat different types of industrial wastewater that are contaminated with heavy metals such as copper. This article focuses on reviewing the most advanced wastewater treatment techniques, including adsorption, membrane filtration, cementation and electrodialysis. The review examines the differences among the treatment methods in terms of duration and overall efficiencies. The review outlines the current research in the area in terms of weaknesses and strengths, leading to future research prospective and pointing out gabs that need to be addressed in future research.

Full text

Review
Copper
removal
from
industrial
wastewater:
A
comprehensive
review
Sajeda
A.
Al-Saydeh
a
,
Muftah
H.
El-Naas
a,
*,
Syed
J.
Zaidi
b
a
Gas
Processing
Center
(GPC),
Qatar
University,
Doha,
Qatar
b
Center
for
Advanced
Materials
(CAM),
Qatar
University,
Doha,
Qatar
A
R
T
I
C
L
E
I
N
F
O
Article
history:
Received
29
June
2017
Received
in
revised
form
18
July
2017
Accepted
20
July
2017
Available
online
27
July
2017
Keywords:
Adsorption
Cementation
Electrodialysis
Heavy
metals
Wastewater
treatment
A
B
S
T
R
A
C
T
Copper
is
one
of
the
most
valuable
and
prevalent
metals
used
in
the
industry.
There
are
many
techniques
to
treat
different
types
of
industrial
wastewater
that
are
contaminated
with
heavy
metals
such
as
copper.
This
article
focuses
on
reviewing
the
most
advanced
wastewater
treatment
techniques,
including
adsorption,
membrane
filtration,
cementation
and
electrodialysis.
The
review
examines
the
differences
among
the
treatment
methods
in
terms
of
duration
and
overall
efficiencies.
The
review
outlines
the
current
research
in
the
area
in
terms
of
weaknesses
and
strengths,
leading
to
future
research
prospective
and
pointing
out
gabs
that
need
to
be
addressed
in
future
research.
©
2017
The
Korean
Society
of
Industrial
and
Engineering
Chemistry.
Published
by
Elsevier
B.V.
All
rights
reserved.
Contents
1Introduction
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35
2
Copper
removal
techniques
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2.1Adsorption
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2.1.1Adsorption
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natural
material
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36
2.1.2Adsorption
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biopolymers
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36
2.1.3Adsorption
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by-products
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2.1.4Adsorption
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low-cost
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2.1.5Adsorption
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nanomaterials
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37
2.2Cementation
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38
2.3Membrane
filtration
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2.3.1Ultrafiltration
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38
2.3.2Nano
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2.3.3
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39
2.4Electrochemical
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2.5Photocatalysis
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3Comparison
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copper
removal
processes
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4Future
prospective
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5Conclusions
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42
References
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42
1
Introduction
The
metal
can
be
classified
as
a
heavy
metal,
if
it
has
a
relatively
high
density
which
is
bigger
than
the
density
of
water
by
five
times
and
if
it
is
toxic
or
poisonous
at
low
concentrations.
Heavy
metals
are
non-biodegradable,
toxic,
and
easy
to
accumulate
at
low
concentrations
in
living
organisms
in
general
and
in
the
human
body
in
specific;
they
can
cause
serious
illnesses,
such
as
cancer,
nervous
system
damage,
and
kidney
failures
and
can
be
deadly
at
high
concentrations
[1–6].
The
most
common
heavy
metals
that
are
often
present
in
industrial
wastewater
include:
nickel,
zinc,
*
Corresponding
author.
E-mail
address:
muftah@qu.edu.qa
(M.H.
El-Naas).
http://dx.doi.org/10.1016/j.jiec.2017.07.026
1226-086X/©
2017
The
Korean
Society
of
Industrial
and
Engineering
Chemistry.
Published
by
Elsevier
B.V.
All
rights
reserved.
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44
Contents
lists
available
at
ScienceDirect
Journal
of
Industrial
and
Engineering
Chemistry
journal
homepa
ge:
www.elsev
ier.com/locate/jie
c

silver,
lead,
iron,
chromium,
copper,
arsenic,
cadmium
and
uranium
[7–10].
However,
copper
is
usually
found
at
high
concentrations
in
wastewater,
because
it
is
considered
as
the
most
valuable
and
commonly
used
metal
in
many
industrial
applications,
such
as
metal
finishing,
electroplating,
plastics,
and
etching
[11–15].
Moreover,
copper
is
a
very
toxic
metal
even
at
low
concentration
and
copper-contaminated
wastewater
must
be
treated
before
discharging
it
to
the
environment
[16–20].
The
permissible
limit
of
copper
ions
in
industrial
effluents
was
reported
by
the
United
State
Environmental
Protection
Agency
(USEPA)
to
be
1.3
mg/L
while
it
was
stated
by
World
Health
Organization
that
copper
ions
content
in
drinking
water
should
not
exceed
2
mg/l
[21–23].
Over
the
past
few
years,
there
have
been
numerous
new
methods
and
techniques
that
were
developed
for
the
removal
of
copper
ions
from
industrial
wastewater,
such
as
adsorption
[24–27],
cementation
[16,28],
membrane
filtration
[29–31],
electrodialysis
[32,33]
and
photocatalysis
[34,35].
This
main
objective
of
this
paper
is
to
review
the
key
options
available
for
copper
removal
and
hence
offer
a
good
start
to
guide
new
researchers
who
want
to
fill
research
gaps
in
the
area
and
improve
the
conventional
copper
removal
methods.
Although
there
are
few
similar
review
papers
dealing
with
the
removal
of
heavy
metals,
they
all
seem
to
be
too
general,
considering
other
metal
ions
or
concentrating
on
a
specific
treatment
method.
To
the
best
of
the
authors’
knowledge,
there
are
no
comprehensive
reviews
published
in
the
open
literature
that
focus
on
the
removal
of
copper
in
spite
of
its
importance
as
a
major
water
contaminant.
Copper
removal
techniques
are
discussed
in
the
following
sections
and
compared
in
terms
of
removal
efficiency,
practicality,
environmental
friendliness
and
process
economics.
2
Copper
removal
techniques
2.1
Adsorption
The
word
“adsorption”
describes
the
process
of
mass
transfer,
where
the
material
is
transferred
from
the
liquid
phase
directly
to
the
surface
of
the
solid
phase,
after
that
it
is
bounded
with
chemical
and/or
physical
interactions
[36].
Davarnejad
and
Panahi
[37]
reported
that
the
adsorption
method
is
considered
to
be
the
most
common
process
used
to
remove
different
copper
ions
from
industrial
wastewater.
Further,
it
provides
many
advantages
compared
to
the
other
treatment
techniques
because
of
the
simplicity
in
design
and
its
ability
to
involve
low
investment
in
terms
of
initial
cost
as
reported
by
Hidalgo-Vázquez
et
al.
[38,39].
On
the
other
hand,
Abdel
Salam
et
al.
[40–42]
reported
some
disadvantages
of
this
process,
such
as
its
limited
applications
to
certain
concentrations
of
copper
ions.
There
are
many
different
low-cost
adsorbents
that
have
been
developed
for
the
removal
of
copper
ions
from
metal-contaminated
wastewater
[43].
These
adsorbents
have
been
derived
from
natural
material,
modified
biopolymers,
biological
wastes,
industrial
by-products,
and
nano-
materials.
2.1.1
Adsorption
on
modified
natural
material
Natural
zeolites
are
the
most
studied
natural
materials
for
the
adsorption
of
heavy
metals
due
to
their
valuable
properties,
such
as
effective
ion
exchange
capability
[44].
Ali
and
YaŞAr
[45]
proved
that
the
clinoptilolite
is
considered
as
one
of
the
most
important
natural
zeolite,
since
it
can
be
found
worldwide.
Also,
it
shows
high
selectivity
for
copper
ions.
Barakat
[46]
studied
the
effect
of
pH
in
this
process,
in
which
the
pH
is
playing
a
main
role
in
the
selective
adsorption
of
varies
copper
ions:
1.
At
natural
pH,
the
NaA
zeolite
is
used
to
remove
Cu(III).
2.
A4
zeolite
is
used
to
adsorb
Cu(II)
at
natural
and
alkaline
pH.
3.
The
adsorption
of
Cu(VI)
is
achieved
at
acidic
pH
using
A4
zeolite.
Clay–polymer
composites
consist
of
natural
clay
minerals,
which
can
be
supported
with
polymeric
material
to
improve
their
capability
of
removing
copper
ions
from
aqueous
solutions
as
reported
by
Azzam
et
al.
[47].
Activated
phosphate
with
nitric
acid,
zirconium
phosphate,
and
calcined
phosphate
at
900

C
are
considered
as
phosphates,
which
have
been
studied
as
a
new
type
of
adsorbents
to
remove
copper
from
wastewater
by
Francis
et
al.
[13,48].
2.1.2
Adsorption
on
modified
biopolymers
Using
modified
biopolymers
adsorbents
is
industrially
attrac-
tive
because
they
have
some
advantages
[49].
For
instance,
they
can
reduce
the
copper
concentrations
in
water
to
sub
parts
per
billion
concentrations,
they
can
be
widely
available,
and
they
are
environmentally
safe.
The
most
attractive
feature
of
biopolymers
is
that
they
contain
different
functional
groups,
such
as
amines
and
hydroxyls,
which
can
increase
the
separation
efficiency
of
heavy
metal
ions
and
make
the
chemical
loading
possibility
reach
the
maximum.
Polysaccharide-based-materials
are
good
example
of
modified
biopolymers,
which
can
be
used
as
adsorbents.
Crini
[50]
reported
that
there
are
two
different
ways
to
prepare
an
adsorbent
that
contains
polysaccharide-based-materials,
which
are:
1.
Crosslinking
reactions,
which
is
the
reaction
that
occurs
between
the
hydroxyl
groups
or
amino
of
the
chains
with
a
coupling
agent
to
form
the
crosslinked
networks
(gels),
which
are
water
insoluble.
2.
Immobilize
the
polysaccharides
on
some
insoluble
supports
by
some
reactions
to
give
hybrid
materials.
2.1.3
Adsorption
on
industrial
by-products
Fly
ash
[51,52],
iron
slags,
hydrous
titanium
oxide,
and
waste
iron
are
industrial
by-products,
which
can
be
chemically
modified
to
improve
their
removal
ability
for
copper
ions
from
industrial
wastewater.
Iron
slag
was
successfully
utilized
to
remove
Cu(II)
ions
at
a
pH
range
of
3.5–8.5
[13],
while
Luo
et
al.
[53]
studied
the
performance
of
fly
ash,
from
the
coal-burning,
for
the
removal
of
Cu(II)
from
aqueous
solutions.
Hydrous
titanium
oxide
has
been
tested
by
Barakat
et
al.
[54,55]
to
adsorb
Cu(II)
and
Cu(VI),
where
the
Cu(II)
adsorption
mechanism
is
achieved
by
surface
hydrolysis
reaction
as
pH
increases.
TiO–Cu(OH)
3
and
TiO–CuOH
+
species
are
examples
of
Cu(II)
complexes,
which
are
considered
as
the
main
products
of
the
surface
hydrolysis
reaction
(Fig.
1).
Fig.
1.
The
adsorption
of
Cu(II)
on
TiO
2
[54].
36
S.A.
Al-Saydeh
et
al.
/
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44

2.1.4
Adsorption
on
low-cost
biosorbents
During
the
past
few
years,
a
considerable
amount
of
research
has
been
devoted
to
the
removal
of
heavy
metals
from
industrial
wastewater
using
adsorbents
that
are
derived
from
agriculture
wastes.
Such
process
is
often
referred
to
as
bio-sorption
[13].
Zeraatkar
et
al.
[56]
reported
that
bio-sorption
is
often
considered
as
one
of
the
most
innovative
technology
for
the
removal
of
heavy
metal
ions
using
non-active
biomass
and
non-living
algae.
Anastopoulos
and
Kyzas
[57]
proved
that
acidic
pH,
between
2
to
6,
is
the
most
effective
range
to
remove
heavy
metals
by
adsorbents
derived
from
modified
biological
wastes.
Further,
it
was
found
that
the
dead
algae
may
have
higher
uptake
of
heavy
metal
ions
as
compared
to
live
algae
by
Ref.
[58].
2.1.5
Adsorption
on
nanomaterials
During
the
past
few
years,
carbonaceous
nanofibers
(CNFs)
and
graphene
oxide
(GO)
have
been
used
to
remove
copper
from
industrial
wastewater.
CNFs
can
be
produced
via
hydrothermal
carbonization
(HTC)
using
any
precursor
such
as
glucose
[59].
The
CNFs
attracted
the
interest
of
many
researchers
because
it
showed
different
advantages
such
as
excellent
mechanical
stability,
good
hydrophilic
nature
and
high
surface
area
[60].
Ding
et
al.
[61]
studied
the
performance
of
CNFs
for
removing
copper
ions
in
multi-component
conditions,
where
copper
ion
was
successfully
adsorbed
on
CNFs
at
acidity
pH.
The
maximum
sorption
capacity
for
Cu
2+
was
found
to
be
204
mg/g
at
pH
5.5

0.2.
Recently,
graphene
oxides
(GOs)
and
GO-based
nanomaterials
have
received
considerable
attention
for
the
removal
of
organic
and
inorganic
pollutants
from
wastewater
due
to
their
unique
properties
such
as
high
surface
area,
large
pore
volume
structure,
chemically
stability,
and
abundant
O
2
-containing
functional
groups
(i.e.
hydroxide
and
carboxyl
groups)
[27,62–67].
Yu
et
al.
[68]
discussed
the
removal
of
copper
ion
using
GO-based
nanomaterial
in
different
composi-
tions,
where
the
maximum
copper
ion
sorption
capacity
was
found
to
be
45.2
mg/g
on
pure
GO.
After
discussing
the
different
types
of
adsorbents,
which
can
be
derived
from
natural
material,
modified
biopolymers,
industrial
by-products,
and
modified
biological
wastes,
the
uptake
rates
at
different
operating
conditions
for
each
adsorbent
have
been
presented
in
Table
1.
These
adsorbents
include
modified
fly
ash,
Table
1
Cu(II)
removal
by
using
different
low-cost
adsorbents.
Type
of
adsorbent
Operating
condition
Uptake
(mg/g)
References
Activated
carbon
prepared
from
Phaseolus
aureus
hulls
(ACPAH)
pH
=
7
20.00
[69]
Activated
carbon
prepared
from
Ceiba
pentandra
hulls
pH
=
6
21.00
[70]
Modified
fly
ash
pH
=
6.4
21.50
[71]
Zeolite
derived
from
fly
ash
pH
=
3.5
147.7
[72]
T
=
310
K
Waste
slurry
pH
=
3
20.97
[73]
Ag
nanoparticle-loaded
activated
carbon
(Ag-NP-AC)
pH
=
4.7
60
[74]
Carbonaceous
nanofibers
T
=
5.5

0.2
204.00
[61]
Live
yeast
(Y.
lipolytica)
pH
=
6.4
204.10
[75]
HCl-treated
clay
pH
=
5
83.30
[76]
Graphene
oxide
pH
=
5
45.20
[68]
Graphene
oxide/Fe
3
O
4
pH
=
5.3
18.26
[77]
T
=
20

C
Treated
fly
ash
with
NaOH
solution
pH
=
6.2
64.00
[78]
T
=
40

C
kaolinite-supported
zerovalent
iron
nanoparticles
pH
=
6.0
49.00
[79]
Bare
NZVI
(FeCl
2

4H
2
O
+
NaBH
4
)
pH
=
6.5
250.00
[80]
MWCNT-reinforced
nanofibrous
matssupported
NZVI
pH
=
5.5
107.80
[81]
Ecklonia
maxima
—
marine
alga
pH
=
6
90.00
[82]
T
=
20

C
Spirogyra
(green
alga)
pH
=
5
133.00
[83]
T
=
22

2

C
Pecan
shells
activated
carbon
pH
=
4.8
31.70
[84]
Amino-functionalization
of
PAA-coated
Fe
3
O
4
nanoparticles
pH
=
5
12.00
[85]
Oligotrophic
peat
pH
=
6.7
12.07
[86]
pH
=
5
06.41
[87]
Eutrophic
peat
pH
=
6.7
12.07
[86]
pH
=
5
19.56
[87]
Iron
oxide
coated
eggshell
powder
pH
=
6
44.00
[88]
Immobilized
nanometer
TiO
2
pH
between
8–9
06.70
[89]
Nanometer
TiO
2
pH
=
8
07.00
[90]
Rose
waste
biomass
pH
=
5
56.00
[91]
T
=
303
K
Valonia
tannin
resin
pH
=
5
44.00
[92]
T
=
298
K
Granular
activated
carbon
pH
=
3
0.79
[93]
Date
pits
pH
=
5.8

0.5
07.40
[94]
Chlorella
vulgaris
pH
between
4–5
01.52
[95]
Chitosan
pH
=
4.5
88.43
[96]
pH
=
5
87.99
[97]
Non-crosslinked
chitosan
pH
=
5
85.00
[98]
T
=
20

C
Crosslinked
chitosan
(EPI)
pH
=
5
62.40
[50]
Crosslinked
chitosan
(TPP)
pH
between
5–6
200.00
[99]
Steel-making-by-product
pH
=
6
40.00
[100]
Scolecite
pH
=
6
04.20
[101]
S.A.
Al-Saydeh
et
al.
/
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44
37

zeolite
derived
from
fly
ash,
treated
fly
ash
with
NaOH
solution,
calcinated
fly
ash,
iron
oxide
coated
eggshell
powder,
granular
activated
carbon,
etc.
2.2
Cementation
Cementation
is
a
general
term
used
to
describe
the
heteroge-
neous
process
in
which
the
copper
ions
in
the
copper’s
salt
solution
(i.e.,
CuSO
4
),
are
reduced
to
zero
valence
at
the
interface
of
iron
by
spontaneous
electrochemical
reduction
to
reach
the
copper
metallic
state,
with
consequent
oxidation
of
the
iron
and
the
dissolved
iron
species
present
more
in
the
aqueous
solution
as
illustrated
in
Fig.
2
[102,103].
The
cementation
process
is
considered
as
the
most
economic
and
effective
technique
to
remove
valuable
and/or
toxic
metals
from
industrial
wastewater
[17].
During
the
past
ten
years,
this
method
has
been
widely
used
in
different
industries
as
a
purification
process
of
industrial
waste
solutions
[16].
Aktas
et
al.
[16,104,105]
studied
the
advantages
of
using
this
technique,
such
as
its
comparatively
low
cost
process
due
to
consuming
low
energy
and
recovering
the
metals
in
pure
metallic
form
with
high
efficiency.
Also,
it
is
easy
to
control
and
it
has
relatively
simple
operation.
On
the
other
hand,
Demirk_
IRan
and
Künkül
[106]
mentioned
the
main
disadvantage
of
cementa-
tion
technique,
which
is
the
excess
sacrificial
metal
consumption.
Wu
et
al.
[107]
proved
that
the
iron
and
zinc
are
the
most
common
cementation
agents
used
in
the
industrial
applications
because
they
have
strong
reductive
ability.
However,
it
seems
that
the
Cu
cementation
using
a
scrap
of
iron,
is
the
simplest
and
most
reasonable
method
for
Cu
recovery
[108].
Therefore,
it
produces
metallic
copper
sediments,
which
are
suitable
for
metallurgical
processes.
The
oxidation/reduction
reactions
are
presented
below
[108]:
Fe
!
Fe
2+
+
2e
Cu
2+
+
2e
!
Cu
The
overall
reaction:
CuSO
4
+
Fe
!
FeSO
4
+
Cu
2.3
Membrane
filtration
Membrane
filtration
has
received
considerable
attention
in
recent
years
for
treating
copper-contaminated
industrial
waste-
water,
since
it
is
applicable
to
remove
suspended
solid,
organic,
and
inorganic
compounds
(i.e.
heavy
metals)
[13].
Furthermore,
Escobar
et
al.
[110–112]
highlighted
the
main
advantages
of
using
membrane
method,
such
as
energy
saving,
no
phase
change,
cost
effectiveness,
easy
to
scale
up,
high
efficiency
in
separation,
and
environmentally
safe.
Several
types
can
be
used
to
remove
copper
ions
from
wastewater,
which
are
classified
based
on
the
particle
size
that
can
be
removed,
such
as
ultrafiltration,
nanofiltration,
and
reverse
osmosis.
However,
Elimelech
and
Phillip
[112]
mentioned
that
further
developments
are
needed
to
improve
the
membrane
filtration
technologies
by
reducing
the
energy
consumption
and
lowering
the
required
thermodynamics
operation
conditions.
2.3.1
Ultrafiltration
Ultrafiltration
(UF)
is
a
promising
membrane
technique
to
remove
copper
ions
from
industrial
wastewater
at
low
transmem-
brane
pressures.
UF
has
a
pore
size
between
5
and
20
nm
and
the
MW
of
the
separated
particles
should
be
within
the
range
(1000–
100,000
Da)
[113,114].
Gunatilake
[113]
proved
that,
based
on
the
characteristics
of
the
membrane,
UF
membrane
can
achieve
a
good
removal
efficiency
(around
90%)
for
initial
copper
concentrations
ranging
from
10
to
160
mg/L,
where
the
best
pH
range
is
from
5.5
to
6
and
at
an
operating
pressure
between
2
to
5
bars.
An
important
advantage
of
UF
is
due
to
the
high
packing
density
which
makes
the
space
requirement
smaller.
Polymer
enhanced
ultrafiltration
(PEUF)
has
also
been
evaluat-
ed
during
the
last
few
years
[113].
PEUF
has
been
proposed
as
a
suitable
method
to
remove
copper
ions
from
industrial
wastewater
(Table
2).
Water-soluble
polymer
is
the
main
type
of
polymer
that
is
used
in
PEUF
process
to
convert
the
heavy
metal
ions
to
macromolecular
complexes,
which
have
a
molecular
weight
that
is
higher
than
the
membrane’s
molecular
weight
cut
off
[115].
There
are
many
parameters
that
play
a
key
role
in
effecting
the
PEUF
process,
such
as
the
metal
to
polymer
ratio,
polymer
type,
and
pH
values.
Finding
the
most
suitable
polymer
that
can
be
used
in
PEUF
process
has
been
the
main
focus
of
many
researchers
during
the
past
few
years.
Fu
et
al.
[114,116]
evaluated
different
types
of
polymers,
which
showed
a
selective
separation
of
copper
ions
with
low
energy
consumption,
such
as
polyethyleneimine
(PEI),
humic
acid,
polyacrylic
acid
(PAA),
and
diethylaminoethyl
cellulose.
Molinari
et
al.
[116]
proved
the
high
efficiency
of
polyethylenei-
mine
(PEI)
in
removing
Cu(II)
from
contaminated
wastewater,
where
the
best
results
were
found
when
the
pH
value
was
above
6
and
the
metal
to
polymer
mass
ratio
was
around
3.
Using
PEUF
process
has
many
advantages
including
high
binding
selectivity
and
high
removal
efficiency.
Although
there
has
been
considerable
amount
of
research
and
many
publications
in
this
area,
PEUF
still
has
not
reached
wide
industrial
applications
[117].
2.3.2
Nano
filtration
The
utilization
of
nanofiltration
(NF)
for
the
removal
of
heavy
metals
has
been
rapidly
increasing
in
recent
years,
since
it
provides
some
critical
solutions
for
certain
problems
associated
with
the
conventional
removal
methods
[120].
Al-Rashdi
et
al.
[121]
proved
the
successful
application
of
NF
membrane
for
heavy
metal
ions
removal.
The
NF
is
considered
to
be
a
pressure
driven
process,
which
has
a
pore
size
between
the
ultrafiltration
(UF)
and
reverse
osmosis
(RO),
and
most
of
NF
membrane
are
charged
with
either
negative
or
positive
charge
[110].
In
addition,
NF
membrane
has
unique
separation
mechanisms,
which
are
Donnan
exclusion
(charge
repulsion)
and
size
exclusion
[110,122,123].
NF
membrane
has
many
advantages
compared
to
the
other
types
of
membrane,
where
it
has
higher
rejection
to
the
multivalent
copper
ions
than
the
UF
membrane
[124].
Further,
compared
to
RO
membrane,
NF
membrane
has
higher
water
permeability
with
relatively
high
rejection
and
much
lower
operating
pressure.
Therefore,
NF
membrane
process
is
considered
as
an
energy-saving
process
that
is
very
effective
for
heavy
metal
ions
removal
[111].
Mohammad
et
al.
[125]
reported
that
the
pore
size
of
the
NF
membranes
is
Fig.
2.
Copper
cementation
on
iron
[109].
38
S.A.
Al-Saydeh
et
al.
/
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44

typically
1
nm
that
corresponds
to
MW
cut-off
(MWCO)
of
300–
500
Da.
There
are
many
different
membrane
processes,
which
were
developed
for
the
selective
separation
to
make
the
initial
cost
lower
and
to
mitigate
the
increasing
concerns
associated
with
heavy
metals
contaminated
wastewater
[114,126].
Kotrappanavar
et
al.
[127]
examined
the
components
of
most
NF
membranes,
which
consist
of
thin
film
composites
made
of
different
artificial
polymers
that
contain
the
charged
groups.
These
groups
can
increase
the
polymers
efficiency
in
the
removal
of
charged
heavy
metal
ions
from
wastewater.
Further,
the
separation
in
NF
achieved
by
electro
migration
as
well
as
sieving,
the
Donnan
effect,
solution
diffusion,
and
dielectric
exclusion,
which
makes
the
NF
mem-
branes
useful
for
the
removal
of
both
uncharged
and
charged
organic
and/or
inorganic
particles.
Al-Rashdi
et
al.
[120]
reported
that
the
NF
membrane
can
recover
almost
100%
of
copper
ions
in
100 0
mg/L
copper
solution
within
a
range
of
pressure
between
3
and
5
bar
and
pH
values
between
1.50
and
5,
which
shows
that
the
suitability
of
NF
membranes
for
copper
ions
rejection.
However,
the
ability
of
NF
membranes
for
copper
ions
rejection
is
decreased
when
the
concentration
of
copper
increased
and
reached
2000
mg/L.
A
comparison
of
Cu(II)
removal
using
appropriate
NF
systems
at
different
operation
conditions
is
presented
in
Table
3.
2.3.3
Reverse
osmosis
Reverse
osmosis
(RO)
is
a
separation
process,
which
uses
applied
pressure
to
force
the
contaminated
wastewater
to
go
through
the
membrane
that
rejects
the
contaminants
on
one
side
and
allows
the
pure
solution
to
go
to
the
other
side
(Fig.
3)
[113].
During
the
past
decade,
RO
has
become
one
of
the
best
separation
technology
for
industrial
wastewater
treatment
for
water
reuse
[128].
The
RO
membranes
often
have
a
thick
barrier
layer
in
the
polymer
matrix
where
most
of
the
separation
process
occurs.
The
RO
process
can
be
used
to
remove
various
types
of
ions
and
molecules
from
different
types
of
contaminated
water,
including
industrial
scale
applications.
However,
the
RO
process
consists
mainly
of
diffusive
mechanisms;
therefore,
the
efficiency
of
the
separation
depends
heavily
on
water
flux
rate,
pressure,
and
solute
concentration
[113].
RO
brine
usually
contains
large
amounts
of
highly
toxic
heavy
metals
(i.e.
Mo,
Cu,
Ni)
and
other
less
toxic
heavy
metals
(i.e.
Zn
and
Fe)
[128].
Tran
et
al.
[128]
reported
that
hybrid
systems,
which
consist
of
electrodialysis
and
a
pellet
reactor
is
the
best
way
for
increasing
the
recovery
of
RO
by
treating
its
concentrate,
where
the
pellet
reactor
removes
scaling
potential
then
the
contaminated
wastewater
is
treated
by
the
electrodialy-
sis.
Many
researchers
investigated
the
efficiency
of
the
RO
process
for
copper
removal
and
found
that
high
separation
efficiency
was
achieved
within
a
range
between
70–99.9%.
Dialynas
and
Diamadopoulos
[129]
tried
to
combine
the
bioreactor
system
and
RO
membranes
together
in
a
pilot
scale
and
found
that
copper
ions
removal
efficiency
was
very
high.
A
summary
of
Cu(II)
removal
using
appropriate
RO
systems
with
different
operation
conditions
is
given
in
Table
3.
2.4
Electrochemical
methods
In
general,
the
electrochemical
removal
methods
have
been
widely
used
in
the
metallurgy
and
metal
finishing
to
separate
the
metal
ions
(i.e.
Zinc,
Copper,
Silver,
Lead)
[114,135,136].
The
most
important
electrochemical
methods
used
for
heavy
metal
ions
removal
are
electrocoagulation
and
electrodialysis.
Electrodialysis
is
considered
to
be
as
an
electrochemical
process
to
separate
copper
ions
from
industrial
wastewater,
where
copper
ions
exchange
through
the
membranes
under
the
electric
field
[32].
Further,
the
electric
field
starts
when
the
reactions
at
the
surface
of
the
electrode
produce
hydroxyl
ions
at
the
cathode
and
protons
at
the
anode.
The
heavy
metal
ions
have
high
affinity
to
be
desorbed
and
transferred
toward
the
cathode
through
the
electromigration
where
the
reason
is
that
the
ionic
transformation
of
the
protons
is
much
higher
compared
to
that
of
hydroxyl
ions
[137].
Ur
Rahman
et
al.
[138]
invented
an
approach
to
reach
an
efficient
and
cost
effective
electrolytic–electrodialytic
apparatus
and
process
for
metal
ions
recovery
from
wastewater
streams.
Fig.
4
represents
the
continuous
flow
of
metal-contaminated
wastewater,
which
can
be
treated
in
flow
battery
of
single
integrated
cells.
Each
single
cell
consists
of
three
main
sections,
which
are
catholyte
section
(101),
metal-contaminated
wastewater
section
(102),
and
anolyte
section
(103).
The
metal-contaminated
wastewater
stream
(100)
will
be
Table
2
Cu(II)
removal
by
PEUF
membrane.
UF
type
Membrane
type
Surfactant
agent
Initial
conc.
Optimum
pH
Removal
efficiency
Reference
PEUF
Polyethersulfone
PEI
50
mg/L
pH
>
6
94%
[116]
PEUF
Polyethersulfone
Carboxy
methyl
cellulose
10
mg/L
pH
=
7
97.6%
[118]
PEUF
Ceramic
Poly(acylic
acid)
sodium
160
mg/L
pH
=
5.5
98-99.5%
[119]
Table
3
Cu(II)
removal
by
using
UF,
NF,
RO,
and
NF
+
RO.
Type
of
membrane
Initial
concentration
Removal
efficiency
Operation
conditions
References
NF
0.01
M
47–66%
Transmembrane
pressure
1–3
bars
[121,130]
NF
0.47
M
96–98%
Pressure
=
20
bars
[131]
RO
7.86

10
3
M
98–99.5%
Pressure
=
5
bars
[128]
RO
Between
4.7

10
4
and
1.57

10
3
M
70–90%
Low
pressure
RO
[132]
RO
+
NF
2
M
More
than
95%
Pressure
=
35
bars
[133]
RO
+
NF
0.015
M
95–99%
Pressure
=
3.8
bars
[134]
Fig.
3.
Reverse
osmosis
mechanism
[113].
S.A.
Al-Saydeh
et
al.
/
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44
39

divided
into
many
streams
that
will
enter
all
cells
from
(108)
and
will
leave
from
(109).
The
metal
ions
will
be
received
by
the
anolyte
section
through
(110)
and
the
produced
oxygen
from
the
anode
will
leave
from
(112)
while
the
produced
hydrogen
from
the
cathode
will
leave
from
(113).
All
effluent
wastewater
will
be
combined
in
stream
(114).
Nasef
et
al.
[135,139]
reported
that
the
properties
of
the
membrane
used
in
the
electrodialysis
process
should
be
taken
into
consideration,
because
these
properties
determine
the
degree
of
copper
ions
separation.
Furthermore,
Caprarescu
et
al.
[140]
studied
the
requirement
of
the
used
membrane
in
electrodialysis
process,
which
should
possess
good
chemical
and
thermal
stability,
where
the
separation
process
can
be
carried
out
at
high
temperatures,
in
a
solution
that
has
a
very
high
or
low
pH
values.
Recently,
the
studies
of
electrodialysis
process
were
mainly
focused
on
the
lab
scale
using
a
3-sections
design
(Fig.
5A),
which
consists
of
a
central
section
that
contains
the
metal
contaminated
wastewater
and
two
neighboring
sections
where
the
electrolytes
are
continually
circulated.
The
experimental
parameters,
such
as
remediation
time
and
current
density
of
the
contaminated
wastewater,
play
a
big
role
to
have
a
good
efficiency
of
heavy
metal
ions
removal
[137].
At
The
University
of
Denmark,
a
new
design
of
electrodialysis
lab
scale
experiments
has
been
developed,
which
consists
of
a
2-sections
cell
(Fig.
5B).
Ebbers
et
al.
[141]
indicated
that
the
use
of
2-sections
cell
in
electrodialysis
remediation
showed
less
performance
compared
to
the
use
of
3-sections
cell.
However,
the
acidification
time
was
significantly
reduced,
the
final
pH
value
was
lower
as
well
as
the
voltage
values
were
lower
in
the
2-sections
cell
compared
to
the
3-sections
cell.
Furthermore,
the
direct
introduction
of
protons
to
the
suspension
was
a
reason
to
make
the
conductivity
higher
in
the
2-sections
cell.
Jensen
et
al.
[142]
introduced
new
design
of
bench-scale
electrodialysis
process,
which
is
electrodialysis
remediation
(EDR)
stack
design
to
improve
the
efficiency
of
the
heavy
metals
contaminated
wastewater
by
reducing
their
leachability.
The
stack
design
consists
of
concentrate
and
feed
sections,
which
have
been
designed
based
on
the
principles
of
the
3-sections
cell
to
make
the
design
suitable
to
scale
up
the
process
to
pilot
plant
[143].
The
contaminated
wastewater
is
continually
circulated
within
the
feed
section,
where
the
concentrate
liquid
is
circulated
through
the
concentrate
section.
As
shown
in
(Fig.
5C),
the
concentrate
and
feed
sections
are
separated
by
the
ion
exchange
membranes,
which
play
an
important
role
in
controlling
the
transfer
of
ions
between
both
sections.
The
acidification
of
the
contaminated
wastewater
is
done
by
the
splitting
of
water
at
the
membrane,
where
the
protons
Fig.
4.
The
principle
of
electrodialysis
cell
used
in
continuous
process
[138].
Fig.
5.
EDR
designs:
A)
3-sections
cell
design
B)
2-sections
cell
design
C)
EDR
stack
design
[107].
40
S.A.
Al-Saydeh
et
al.
/
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44

are
accumulated
at
the
feed
section.
However,
the
separated
heavy
metal
ions
are
transported
from
the
feed
section
to
the
concentrate
section
by
electromigration
[137].
Many
researchers
[144–146]
have
reported
that
electrocoagu-
lation
is
a
suitable
technology
for
heavy
metals
removal,
including
Cu,
from
industrial
wastewater
streams.
Electrocoagulation
is
one
of
the
electrochemical
approaches,
which
can
use
electrical
current
to
remove
copper
ions
from
industrial
wastewater
[147].
It
is
based
on
the
generation
of
coagulant
in
situ
by
dissolving
a
metal
anode
from
Al,
Fe
or
hybrid
Al/Fe
electrodes
[148].
The
generation
of
metal
ions
takes
place
at
the
anode,
while
hydrogen
gas
is
released
from
the
cathode,
which
can
help
to
float
the
particles
that
are
flocculated
out
of
the
water.
Electrocoagulation
has
many
advantages
over
other
treatment
methods;
it
is
fast,
simple,
inexpensive,
easy
to
operate
and
environmentally
safe
[149,150].
The
current
density
is
the
most
important
parameter
in
the
electrocoagulation
process,
in
which
it
can
determine
many
factors
such
as
the
bubble
production
rate,
the
coagulant
dosage
rate,
and
the
size
and
growth
of
the
flocs;
the
efficiency
of
electrocoagulation
can
be
affected
by
these
factors.
The
anode
dissolution
rate
is
often
increased
when
the
current
density
increases,
which
leads
to
increasing
in
the
number
of
copper
hydroxide
flocs
that
results
in
increasing
in
copper
removal
efficiency
[151,152].
The
effects
of
the
operation
mode
(batch
or
continuous),
electrode
material,
current
or
current
density,
optimum
pH,
conductivity
of
the
solutions,
energy
consumption
on
the
copper
removal
efficiency
in
the
electrocoagulation
process
are
shown
in
Table
4.
In
spite
of
the
considerable
amount
of
research
and
process
developments
in
electrocoagulation
technology
over
the
past
decade,
further
research
is
still
needed
to
study
the
effect
of
cell
design
and
electrode
geometry
on
the
efficiency
of
heavy
metal
removal.
Further,
most
of
the
current
studies
have
been
carried
out
at
the
laboratory
scale,
and
hence
more
efforts
should
be
made
to
evaluate
the
electrocoagulation
process
at
pilot
plant
scale.
2.5
Photocatalysis
Photocatalysis
is
a
promising
method
for
the
treatment
of
several
types
of
industrial
wastewater.
In
this
process,
the
electron–hole
pairs
(e

/h
+
)
can
be
continuously
generated
from
semiconducting
under
solar
radiation.
Many
different
semi-
conductors
have
been
used
such
as
ZnS,
ZnO,
TiO
2
,
CdS,
and
CeO
2
[159].
Different
studies
have
been
reported
in
the
literature
to
find
the
most
suitable
semiconductor
for
copper
removal.
Mahdavi
et
al.
[160]
reported
that
TiO
2
is
the
most
widely
used
because
of
its
high
photocatalytic
activity,
high
stability,
nontoxicity,
and
excellent
dielectric
properties.
The
photocatalysis
process
to
remove
Cu(II),
using
TiO
2
as
a
semiconductor
and
a
254
nm
UV-
C
lamp
at
different
experimental
conditions,
has
been
reported
[161].
The
best
results
for
the
removal
of
Cu(II)
was
achieved
at
pH
within
a
range
3.5–4.5
and
TiO
2
mass
between
0.5
and
0.75
g.
The
results
indicate
that
the
TiO
2
can
be
used
in
the
photocatalysis
process
to
remove
around
80%
of
Cu(II)
[160,161].
Moreover,
Barakat
et
al.
[162]
conducted
an
experiment
on
the
photocatalytic
degradation
using
UV-irradiated
TiO
2
suspension
for
the
removal
of
copper
and
destroying
the
complex
cyanide.
The
obtained
results
show
that
copper
with
initial
concentration
=
10
2
M
was
completely
removed
within
3
h.
Wahyuni
et
al.
[163]
studied
the
photocatalytic
removal
of
Cu(II),
where
the
process
was
carried
out
with
an
initial
concentration
of
10
mg/L
using
TiO
2
with
UV
lamp
having
a
wavelength
within
a
range
of
290–390
nm.
The
maximum
photocatalytic
efficiency
was
reached
when
using
50
mg
of
TiO
2
at
pH
5;
about
45.56%
of
the
copper
ions
were
removed.
3
Comparison
of
copper
removal
processes
Generally,
many
different
methods
have
been
studied
by
larger
number
of
researchers
to
remove
copper
ions
from
industrial
wastewater.
These
treatment
methods
can
be
classified
as
chemical,
physical,
and
biological,
and
they
are
often
selected
based
on
many
advantages
such
as
high
selective
separation,
simplicity
in
control,
and
lower
space
requirement.
Physico-
chemical
treatments
can
be
considered
to
be
the
most
suitable
treatment
methods
for
the
removal
of
copper
ions
from
industrial
wastewater.
However,
they
still
suffer
from
high
operating
cost
due
to
the
high
cost
associated
with
the
chemicals
used
and
high
energy
consumption.
Since
metal-contaminated
wastewater
may
contain
some
inorganic
and
organic
matters,
photocalatysis
is
a
promising
method
for
the
removal
of
organic
and
inorganic
contaminants
together.
Overall,
each
treatment
method
has
its
own
advantages
and
limitations.
Table
5
summarizes
the
main
advantages
and
disadvantages
of
the
different
physico-chemical
treatments,
which
have
been
discussed
in
this
review.
4
Future
prospective
Water
treatment
for
the
removal
of
heavy
metals
has
seen
considerable
success
in
recent
years
and
witnessed
vast
develop-
ment
in
applications
and
technologies.
However,
more
research
is
still
needed.
Future
studies
on
copper
removal
should
focus
on
the
interaction
mechanism,
especially
on
the
molecular
level
such
as
X-ray
photoelectron
spectroscopy
(XPS),
X-ray
absorption
fine
structure
(XAFS),
transmission
electron
microscopy
(TEM),
X-ray
diffraction
(XRD),
and
Fourier
transform
infrared
spectroscopy
(FT-
IR)
[167–169].
Recently,
these
methods
have
been
applied
in
order
to
investigate
and
study
the
adsorption
mechanism
[170].
XAFS
spectroscopy,
including
X-ray
absorption
near
edge
structure
(XANES)
spectroscopy
and
extended
X-ray
absorption
fine
structure
(EXAFS)
spectroscopy,
has
the
ability
to
provide
the
microstructure
information
of
radionuclides
[171,172].
Bond
distances,
oxidation
state,
and
coordination
numbers,
which
are
the
main
examples
of
microstructures
of
copper
ions
that
have
been
adsorbed
on
the
adsorbent
surfaces
at
molecular
level,
can
be
calculated
from
the
measurement
and
analysis
of
EXAFS
spectros-
copy
[173].
The
interaction
mechanism
can
then
be
estimated
from
Table
4
Different
systems
for
Cu(II)
removal
by
electrocoagulation
process.
Reactor
Current
density
Conductivity
(mS/cm)
Energy
consumption
Optimum
pH
Electrode
materials
Removal
efficiency
References
Continuous
4.8
A/dm
2
–
–
4
Al–Al
99%
[153]
5
A
–
10.99
kWh/Kg
0.64
Ss–Ti
98.8%
[154]
Batch
5
A
1.600
35.63
kWh/g
7
Fe–Fe
99.99%
[155]
5
A
1.600
35.06
kWh
7
Al–Al
99.9%
[150]
0.3
A
0.634
–
5
RO–Ti–Ss
99%
[156]
100
A/m
2
2
10.07
kWh/m
3
3
Fe–Al
100%
[157]
33
A/m
2
20
–
9
Al–Al
>50%
[158]
S.A.
Al-Saydeh
et
al.
/
Journal
of
Industrial
and
Engineering
Chemistry
56
(2017)
35–44
41

the
information
of
the
bond
distances
and
coordination
number,
which
can
be
obtained
from
EXAFS.
5
Conclusions
The
removal
of
heavy
metals
in
general
and
copper
from
industrial
wastewater
is
a
very
important
part
of
most
of
the
current
research
in
the
environmental
field,
due
to
the
harmful
effects
of
heavy
metals
on
the
human
health
and
living
organisms
in
the
environment.
Different
treatment
methods
such
as
physical,
chemical
and
biological
methods
have
been
discussed
in
this
review
paper,
which
considered
studies
encompassing
the
past
fifteen
years.
These
methods
include
adsorption,
cementation,
membrane
filtration,
electrodialysis,
and
photocatalysis.
However,
it
is
important
to
note
that
the
selection
of
the
most
suitable
method
depends
on
some
parameters
such
as
economic
parameter
(i.e.
operation
cost),
environmental
impact,
initial
concentration
of
the
copper
ions,
pH
values,
and
the
overall
performance
of
the
method
compared
to
the
other
methods.
Finally,
more
research
work
is
still
needed
for
each
method
to
improve
it
and
make
it
more
efficient.
For
the
adsorption
method,
using
biosorbents
to
treat
wastewater
is
a
relatively
new
process
and
studies
in
this
area
are
limited;
therefore,
new
types
of
biosorbents
are
needed
to
be
tested
to
reach
the
maximum
efficiency.
In
cementation,
the
current
cementation
agents
take
time
to
reduce
higher
copper
ions
from
the
wastewater;
therefore,
future
research
in
the
areas
should
be
focused
on
testing
new
cementation
agents
that
can
reduce
the
process
time.
Further,
the
effect
of
pressure
as
an
operating
parameter
has
not
been
evaluated.
For
membrane
filtration,
innovative
techniques
are
needed
for
the
development
of
inexpensive,
easily
available,
superior
and
long
lasting
membranes.
As
for
electrodialysis,
the
development
of
new
designs
is
necessary
to
improve
the
separation
efficiency.
Finally,
more
studies
on
the
effect
of
temperature
are
needed
in
the
photocatalysis
method.
Development
of
catalysts
for
a
high
photo-efficiency
process
that
can
utilize
wider
solar
spectra
is
needed.
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Removal
method
Advantages
Disadvantages
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Adsorption
using
low-cost
adsorbents

Low
initial
cost

Simple
design

limited
to
certain
concentrations
of
copper
ions
[36,37]
Cementation

Low
cost
process

Consumes
low
energy

Easy
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control
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simple
operation

Excess
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Membrane
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Highly
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High
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Electrochemical
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Eco-friendly
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High
operating
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
High
energy
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Photocatalysis

Removal
of
organic
and
metals
contaminants
together

Produces
less
toxic
by-products

The
duration
time
is
long

It
has
limited
applications
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