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Article history:
Received 13 April 2015
Received in revised form
2 November 2015
Accepted 2 November 2015
Available online 12 November 2015
Acid mine drainage (AMD) presents serious threats to the environment due to its toxic constituents.
Traditional wastewater treatment methods such as neutralization, precipitation, membrane processes,
ion exchange and biological sulphate removal, etc., have been applied to remediate AMD and reduce its
negative impact on the receiving environment. However, the challenge with most of these methods is
that the constituents of AMD have not been viewed as valuable resources. The constituents, though toxic
can be recovered and transformed into valuable materials which could be marketed. Amongst the
various AMD constituents, is sulphuric acid which has an appreciable market in the chemical and
metallurgical industry. The acid value could be recovered from AMD and used to meet the demands of
various sulphuric acid consumers. The nancial benets obtained could then be used to offset the overall
AMD treatment cost. Hence, this paper reviews some of the techniques used to recover sulphuric acid
from various wastewater solutions. The techniques reviewed include: rectication, membrane separation, solvent extraction, crystallization and acid retardation. The technical and economic feasibility of
each process for application to AMD is also evaluated. Subsequently, the acid retardation and crystallization technologies are recommended as the most promising technologies for acid recovery from AMD.
2015 Elsevier Ltd. All rights reserved.
Keywords:
Acid mine drainage
Sulphuric acid
Wastewater treatment
Environmental effect
Contents
1.
2.
3.
4.
5.
6.
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
Occurrence and composition of acid mine drainage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
Utilization of sulphuric acid . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
Recovery of sulphuric acid . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
4.1.
Rectification process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
4.2.
Membrane processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
4.3.
Solvent extraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
4.4.
Crystallization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
4.5.
Acid retardation process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
Economic evaluation of the proposed processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
Summary and future prospects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
Disclaimer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
1. Introduction
18
(1)
In sufciently oxidising environment (dependant on O2 concentration, pH greater than 3.5 and bacterial activity) the ferrous
iron released in Reaction 1 may be oxidised to ferric iron, according
to the following reaction (Blowes et al., 2003; Ackil and Koldas,
2006).
(2)
(3)
19
Table 1
Applications of sulphuric acid.
Application
References
Leaching
Electroplating
Acid pickling
Steel making
Automobile batteries
Paper bleaching
Fertilizers
Gasoline
Sugar bleaching
Water treatment
Sulphonation agent
Colouring agent
Amino acid intermediates
Regeneration of ion exchange resins
Cellulose bres
Pharmaceuticals
McDonald and Whittington, 2008; Venter and Boylett, 2009; Zhao et al., 2014
Hudson, 1994
Parujen, 1997, Sheedy, 1998
Martin, 2014
ATSDR, 1998
Martin, 2014
ICF, 2012; Hudson, 2012; IHS, 2014
Hudson, 2012
Manzoor et al., 2012
Inyo, 2013
ATSDR, 1998
HSBD, 2010
ICF, 2012
Robinson et al., 1998
Manzoor et al., 2012
Hudson, 2012
20
Table 2
Summary of methods used for sulphuric acid recovery.
Method
Solution content
H2SO4 recovery
Advantages
Disadvantages
References
Rectication
H2SO4, nitro
compounds
H2SO4, Al
H2SO4, Fe, V
H2SO4, Ni
H2SO4, rare earth
sulphates
H2SO4, Ni
H2SO4, Fe
H2SO4, Cu, Sb, As
H2SO4, Fe, Na
H2SO4, Fe
H2SO4, Fe
H2SO4, Ni
H2SO4, Fe
R 98.3%
Diffusion dialysis
Electrodialysis
Acid retardation
Crystallization
Solvent extraction
H2SO4, Cu
H2SO4, Fe, Mn
H2SO4, Zn
R
R
R
R
R
R
R
e
R
R
R
82e90%
84%
80%
70e80%
80e90%
90%
Up to 99%
74e96%
96%
70e95%
E 75e79%
E 90%
E 90%
Vapour
Heated
solution
Pre-filtered
AMD
Boiler unit
Cooling tower
Recovered
water
Clean H2SO4
output
Fig. 1. Proposal ow diagram for the recovery of sulphuric acid from acid mine drainage using rectication process.
reported low pay back periods for diffusion dialysis, ranging from
slightly over a year to 27 months (Lin and Lo, 1998; Jeong et al.,
2005) making the method economically attractive.
Electrodialysis has also been studied for the recovery of acid
from waste solutions. As already indicated, perm-selectivity is
supported by use of an electric eld. Several studies on the recovery
of organic acids from waste solutions have been published, e.g.,
tartaric acid (Audinos and Paci, 1992), glutonic acid and lactic acid
(Yu et al., 2003; Novalic et al., 2000), etc. Yu et al. (2003) also found
that, apart from many other factors which can be determined
experimentally, the concentration of the recovered organic acid
was mainly inuenced by the current density. Thus, by optimizing
the current density, it is possible to obtain high organic acid concentrations from waste solutions. The recovery of inorganic acids
has also been studied. Ali et al. (2004) recovered nitric acid from
ammonium nitrate solutions. High purity sulphuric acid and sodium hydroxide were obtained from an aqueous sodium sulphate
solution using a three-compartment redox potential (Eh) cell
(Tzanetakis et al., 2002). However, the operating cost of the process
was high compared to the method that used a two-compartment
cell. Cattoir et al. (1999) also found that 90% of the sulphuric acid
present in stainless steel decontamination waste could be recovered using the electrodialysis method. Sulphuric acid recovery from
an acidic nickel sulphate solution (Baltazar et al., 1992), copper
containing solutions (Cifuentes et al., 2006) and recently AMD
(Mart-Calatayud et al., 2013) has also been studied. MartCalatayud et al. (2013) found that an effective recovery of sulphuric acid with no Fe3 species present was obtained in the anodic
compartment as a result of the co-ion exclusion mechanism in the
membranes. This is a very promising technology for acid recovery
from AMD due to its ability to produce high purity acid. However,
the performance of the process with respect to real AMD solution
containing various heavy metal ions still remains to be explored.
Furthermore, the formation of precipitates at the surface of the
membrane related to an abrupt increase in cell voltage was found to
limit the process performance (Mart-Calatayud et al., 2013).
Membrane distillation is one of the most promising membrane
technologies for the recovery of acids (Tomaszewska et al., 1995,
1998, 2000; Tang and Zhou, 2006; Tomaszewka and Mientka,
2009; Wang and Chung, 2015). It involves the use of a hydrophobic membrane which separates two aqueous solutions at different
temperatures and composition to get a concentrated solution
containing the acid and the salts. As a result, fresh water and
concentrated acid or salt are obtained. Membrane distillation is
considered a highly selective operation for both non-volatile
(Regel-Rosocka, 2010) and volatile (Tomaszewka et al., 2000) solutions. It also offers advantages of low energy consumption, high
efciency and operation at low temperatures to recover fresh water
and concentrate the acid and metals (Tomaszewska et al., 1998,
2001). However, the process has been mostly tested at laboratory
scale and its success in the recovery of sulphuric acid from industrial efuents still needs further investigation.
Membrane electrolysis has been investigated for the recovery of
acids from waste solutions. For example, high purity hydrochloric
De-ionized water
Pre-filtered AMD
solution
Clean H SO product
Fig. 2. Proposal ow diagram for the recovery of sulphuric acid from acid mine
drainage using diffusion dialysis method.
21
H SO product
Pre-filtered AMD
solution
Electrodialysis unit
Fig. 3. Proposal ow diagram for the recovery of sulphuric acid from acid mine
drainage using electrodialysis method.
acid has been recovered from spent pickling liquors using a combination of ion exchange and membrane electrolysis (Csicsovszki
et al., 2005). In this study, zinc was recovered in the rst step using anion exchange and the acid recovered in the second step by
membrane electrolysis. The process also appears to be a prospective technique for the recovery of sulphuric acid from waste solutions due to its simplicity and ability to signicantly reduce solid
waste. However, the evolution of hydrogen gas at the cathode was
noted as a drawback to this process (Csicsovszki et al., 2005).
Furthermore, the high cost associated with the energy demand of
the process could reduce interests in exploring the technology
further.
Figs. 2 and 3 are proposed ow diagrams for the recovery of acid
from AMD using diffusion dialysis and electrodialysis, respectively.
In both ow diagrams, the pre-ltered AMD solution is passed
through a membrane unit where a clean acid and an acid barren
water product can be obtained. In general, it can be seen that most of
the membrane separation processes are environmentally attractive.
Apart from signicantly reducing the solid waste, high purity acid
product can be obtained in most cases. Nevertheless, the high capital
cost as well as the running cost associated with heating the solutions
and membrane replacement (due to fouling) might be too high to
make it economically viable for AMD treatment. Furthermore, since
sulphuric acid is well known to be the cheapest inorganic acid
available, the revenue realized from the sale of the product might be
too low to compensate for the overall treatment cost. The development of new membranes which can possibly compensate for high
cost by having high permeability and less fouling could nd their use
in AMD more justiable. Furthermore, reducing costs by employing
low cost energy sources such as solar or wind to drive processes like
electrodialysis could promote their use.
22
AMD solution
Extraction stages at
ambient temperature
Recovered H SO
Stripping stages at
ambient temperature
Raffinate
Stripped extractant
Stripping agent
Fig. 4. Proposal ow diagram for the recovery of sulphuric acid from acid mine drainage using solvent extraction method.
Pre-filtered
AMD solution
23
FeSO4. 7H2O
crystals
Reactor and crystal settler
unit
Centrifuge unit
Chilled H2SO4
product
Fig. 5. Proposal ow diagram for the recovery of sulphuric acid from acid mine drainage using freeze crystallization technology.
Concentrated
acid solution
Acid barren
water
AMD
Acid retardation
system
Diluted acid
solution
Vacuum
evaporator
Re-usable water
Elution water
Fig. 6. Proposed acid retardation set up for sulphuric acid recovery from acid mine drainage.
24
Table 3
Assumptions used in the economic evaluation calculations.
Description
Units
Value
Hour/year
Hour/year
Hour/year
Litre/hour
%
$/tonne
$/tonne
8760
1560
7200
1500
95
560
130
70% and market it to consumers requiring such levels of acid concentration. The benets derived from this proposed process not
only include reduction in energy required for evaporation, but
production of a marketable grade of sulphuric acid. Nevertheless,
research is required to test the feasibility of the proposal ow sheet
for acid recovery.
5. Economic evaluation of the proposed processes
To establish sustainability assessment, an economic evaluation
of the proposed processes is essential. Therefore, a conceptual
economic evaluation of the proposed processes was conducted
based on cost information of available plants. The assumptions
used in the calculations are summarized in Table 3.
The capital and operating costs in the order of magnitude were
estimated using the sixth tenth rule (Equation (5)).
Cf C1
S2
S1
0:6
(5)
Table 4
A summary of capital and operating expenditures of proposed process routes.
Cost (US$)
Rectication
Diffusion dialysis
Electrodialysis
Solvent extraction
Crystallization
Acid retardation
1 193 165
1 372 140
427 789
z9800
381 780
439 047
247 752
z9800
1 523 478
1752 000
266 809
z9800
442 956
509 399
125 124
z9800
407 268
468 368
154 798
z10 320
307 973
354 169
124 810
z9800
25
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