1/28/24, 9:48 PM Separation of mercury from its aqueous solution through supported liquid membrane using environmentally benign

ly benign diluent - S…

Journal of Membrane Science

Volume 350, Issues 1–2, 15 March 2010, Pages 395-401

Separation of mercury from its aqueous solution through

supported liquid membrane using environmentally benign
diluent
Kabita Chakrabarty, Prabirkumar Saha, Aloke Kumar Ghoshal

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https://doi.org/10.1016/j.memsci.2010.01.016
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Abstract

This paper presents an experimental investigation on the facilitated transport of mercury through flat sheet supported
liquid membrane (SLM) containing trioctylamine (TOA) as carrier and coconut oil, an environmentally benign solvent,
as diluent. Co-transport mode of mercury transfer was studied using aqueous solution of NaOH as the strip phase.
Various polymeric supports were tested in order to select the best SLM configuration. The SLM combination “PVDF–
TOA–coconut oil” shows encouraging results and it was stable for a period of 98 h. The fundamental parameters, such
as feed phase pH and concentration, strip phase concentration, carrier concentration, etc., affecting the transfer of
mercury through the SLM were studied. It was observed that the extraction of mercury increases with increase in
NaOH concentration in the strip phase, and becomes steady at a 0.3 M NaOH. The extraction process depends on feed
phase pH and maximum extraction was achieved at a pH of 1. The carrier concentration had marginal effect on
extraction as about 91% separation of mercury was achieved without any carrier in the SLM. Even at the most
favourable operating condition (viz., 0.3 M NaOH, 4% TOA and pH 1), extraction of mercury was achieved up to 95%.
Coconut oil showed better performance in the separation of mercury compared to other organic solvents such as
dichloroethane and heptane.

Introduction

Mercury poisoning is a global concern due to its highly toxic, carcinogenic and non-biodegradable nature. The major
sources of mercury pollutions are the waste of various industries such as chloro-alkali, rubber processing, fertilizer,
battery, pulp and paper, mining, combustion, etc. Even agricultural waste contributes to the mercury pollution to a
considerable extent. Among the various forms of mercury, Hg2+ is the most toxic one as it can easily bind with protein
and cause severe health hazards. Moreover, mercury can form methyl mercury through abiotic and biotic methylation
and this organic ion of mercury is more toxic than inorganic ion of mercury. Because of its highly toxic and
carcinogenic nature, mercury is included in the list of priority pollutants by the US EPA [1]. The permissible level of
mercury in drinking water and wastewater is restricted to 1 and 5 μg l−1, respectively, by the European environmental
regulations [2]. Hence, development of an effective mercury separation method is a matter of great environmental
importance.

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1/28/24, 9:48 PM Separation of mercury from its aqueous solution through supported liquid membrane using environmentally benign diluent - S…

The typical concentration of mercury, as found in various sources of industrial wastewater, is about 10 mg l−1 [3].
Though conventional methods such as precipitation, coagulation, electrodialysis, adsorption, solvent extraction,
chemical oxidation and reduction and ion exchange have been used for mercury separation [4], [5], liquid membrane
(LM) based separation process promises an effective separation of metal ions when the amount of ion in the solution is
trace [6]. Liquid membrane (LM) in general is a homogeneous, non-porous, thin film of organic liquid interposed
between two aqueous phases of different compositions. The solute is transferred from one aqueous phase to another
phase across the LM due to concentration gradient. LMs are generally of two types, viz., supported (SLM) and non-
supported (non-SLM). When a hydrophobic porous membrane support is impregnated with the said organic liquid,
and the saturated support interposes between the two aqueous phases, the total configuration is called a supported
liquid membrane (SLM). The components of the aqueous solutions can move through this LM/SLM from one phase to
the other by means of diffusional process.

Many research groups have studied the LM based processes for the separation of mercury from various aqueous media.
They have used several combinations of diluent–carrier such as chloroform–microcyclic ligands [7], dichloromethane–
calixarene nitril [8], n-paraffins–oleic acid [9], chloroform–tetrathia crown-4 [10], dichloroethane–methyl red [11],
toluene–trioctylamine [12] and nitrophenyloctyl ether–tetrathia-12-crown-4 [13] for the above purpose. About 80–
100% separation of mercury was achieved in the above cases. Most of the above LM based processes were non-SLM. On
the other hand, SLM is advantageous over its non-SLM counterparts because of its simplicity in construction and
operation [14], [15].

From the literature reported above, it was observed that most of the LM based processes used organic solvents as the
diluents. One common problem, seldom encountered with SLM, is the instability of the membrane due to loss of liquid
that oozes out from the membrane pores. Organic solvents are generally volatile in nature and they do have some
degree of toxicity. The volatility of the solvent thereby increases its loss and that eventually makes the SLM more
unstable. Moreover, the toxicity due to the strayed solvent is never desirable for obvious reasons. Thus, it is essential to
look for environment-friendly solvent for successful operation of SLM based unit. Vegetable oils are ideal replacement
for the conventional volatile organic diluents. These oils are less volatile and non-toxic in nature. Very few literatures
are available on the use of vegetable oil as diluent in LM processes. Separation of dyes and copper through SLM has
been reported [16], [17] where vegetable oils such as palm oil, sunflower oil and coconut oil were used as diluents.
Coconut oil has been observed to be stable diluent for the separation of Cu2+ from copper plating wastewater and
about 60–70% removal of copper could be achieved.

The aim of the present work is to explore the feasibility of using coconut oil as a diluent in SLM for the removal of
mercury. This research group, in its previous reports [14], [15], has substantiated the use of TOA as an efficient
extractant (carrier agent) for LM process. In this study, coconut oil and TOA are used as diluent and extractant,
respectively, for the separation of mercury from its aqueous solution through SLM. An experimental investigation was
carried out to describe the performance of coconut oil in the separation of mercury as diluent. Various polymeric
support materials such as polyethylene (PE), polytetrafluroethylene (PTFE), polyvinyldenefluoride (PVDF), Nylon 6,6,
etc., were tested to select a suitable support for the SLM. The fundamental parameters, such as feed pH and
concentration, strip phase concentration, carrier concentration and feed to strip ratio, that affect the transport of
mercury through the SLM were investigated. Moreover, the stability of the SLM was tested and finally, the performance
of coconut oil was compared with two other organic solvents, viz., dichloroethane and heptane.

Section snippets

Chemicals and reagents

All reagents used in this experiment were of GR grade. Aqueous solutions were prepared by using Milli-Q® de-ionized
water (Millipore®, USA). Mercury chloride (HgCl2) was obtained from Merck (India). Parachute coconut oil was
obtained from Marico India limited (India) and TOA was procured from Merck® (Germany). All other chemicals such as
1,2-dichloroethane, hydrochloric acid (HCl), sodium hydroxide (NaOH), stannous chloride (SnCl2) and nitric acid
(HNO3) were obtained from Merck® (India).

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1/28/24, 9:48 PM Separation of mercury from its aqueous solution through supported liquid membrane using environmentally benign diluent - S…

The…

Choice of support material

The efficiency of various polymeric supports (Table 1) soaked with LM was studied through a series of experiments. In
each experiment, the initial concentration of Hg2+ in feed phase was 10 mg l−1 and its pH was 1.5. The concentration of
TOA in the LM was 4% (v/v) and concentration of NaOH at the strip phase was 0.1 M. Each experiment was run for 3 h.
The results are shown in Fig. 1. The separation of mercury is maximum with PTFE (0.2 μm) followed by PTFE (0.45 μm).
PVDF, PE and Nylon 6,6 yield…

Conclusion

The feasibility of an LM based mercury removal process using an environmentally benign diluent, viz., coconut oil, has
been investigated in this work. A batch SLM experiment is carried out in co-transport mode. The fundamental
parameters affecting the transport of mercury through SLM are investigated to obtain the best operating conditions
that would yield maximum separation of mercury from its aqueous solution. The SLM combination “PVDF–TOA–
coconut oil” offers the best result in the separation …

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