- Title
- Performance of magnetic nanocomposites for the removal of some selected contaminants from aqueous solution
- Creator
- Ojemaye, Mike Onyewelehi
- Subject
- Nanocomposites (Materials)
- Date
- 2017
- Type
- Thesis
- Type
- Doctoral
- Type
- PhD
- Identifier
- http://hdl.handle.net/10353/8746
- Identifier
- vital:33508
- Description
- In this thesis, the performances of magnetic nanoparticles based materials were assessed for the removal or reduction of heavy metals in aqueous solutions. The successful synthesis of a novel adsorbent, azomethine functionalized magnetic nanoparticles (MNP-Maph) by covalent bonding between the amine group (-NH2) of amine functionalized magnetic nanoparticles (MNP-NH2) and carboxylic group (-COOH) of 4-{[(E)-phenylmethylidene]amino}benzoic acid (Maph-COOH) was achieved. This adsorbent was examined for the removal of di and trivalent ions (Cu2+, Zn2+, As3+, Pb2+ and Hg2+) from aqueous solutions. Also, magnetic photocatalyst with silica interlayer (NiFe2O4-SiO2-TiO2) was synthesized and employed for the reduction of Cr(VI) in aqueous solution. The photocatalytic reduction efficiency of this material was compared with that of magnetic titanium dioxide (NiFe2O4-TiO2) photocatalyst and titanium dioxide (TiO2) to ascertain the material with the best photocatalytic efficiency and ease of separation. All synthesized materials were characterized by using XRD, FT-IR, TEM, SEM, TGA and VSM before application. For the adsorption processes, the effects of pH, contact time, adsorbent dose and temperature were examined to ascertain the experimental condition necessary for the optimal removal of metal ions from solution. The data obtained from all experiments were fitted into four kinetic models; pseudo-first order, pseudo-second order, elovich and intra particle diffusion models to determine the mechanism involved in the adsorption of these di and trivalent ions while two isotherm models were employed in the adorption processes; these include: Langmuir and Freudlich models. Also, for the photocatalytic experiment, the effects of pH, contact time and photocatalyst dose were investigated to determine the experimental conditions necessary for the optimal reduction of Cr(VI) in aqueous solution. MNP-Maph showed excellent removal capacities of 34.08, 35.83, 50.08, 58.24 and 59.24 mg g-1 for Cu2+, Zn2+, As3+, Pb2+ and Hg2+ respectively compared to data previously reported in literature. This is as a result of the high affinity of azomethine group towards metal ions which tremendously enhanced removal of metal ions by adsorption. The incorporation of azomethine to magnetic nanoparticles improved the affinity towards metal ions removal forming strong electrostatic interaction between the adsorbent active sites and adsorbates. Also, the utilization of NiFe2O4-SiO2-TiO4, NiFe2O4-TiO2 and TiO2 for the reduction of Cr(VI) in aqueous solution showed a good photocatalytic performance with NiFe2O4-SiO2-TiO2 showing to be better in terms of both photocatalytic reduction and magnetic separation. TiO2 was observed to have 96.7percent reduction efficiency within 240 min while NiFe2O4-SiO2-TiO2 has 96.5percent reduction efficiency within 300 min and NiFe2O4-TiO2 gave 60percent reduction efficiency within 300 min of UV irradiation. This magnetic photocatalyst composite (NiFe2O4-SiO2-TiO2) gives the advantage of avoiding the problem of separation often encountered with most photocatalyst materials including TiO2 by allowing separation with the aid of a magnetic field. The adsorption processes were all described by pseudo-second order and Langmuir isotherm models while the photocatalytic process was described by Langmuir-Hinshelwood (L-H) kinetic model. Furthermore, thermodynamic experiment studied for the adsorption processes showed that all metal ion adsorption except Hg2+ by MNP-Maph were endothermic in nature, rapid and spontaneous indicating the feasibility of the sorbent material for the removal of metal ions from aqueous solutions. Also, regenerability study conducted to determine the reusability of sorbent material after seven cycles showed the potential to reuse sorbent material seven times or more. The reusability of the sorbent material was observed to show a percentage of an average of 78percent using 50:50 mixture of 0.1 mol dm-3 HNO3 and HCl for all adsorption processes. For the photocatalytic experiment, regenerability using 0.1 mol dm-3 for 1 h was observed to be very impressive after 3 runs for all synthesized photocatalytic materials. This thereby implies that the removal of metal ions by these materials will not in any way introduce secondary pollutants into the environment. Rather, it will avert the production of secondary pollutants. Also, the use of simple conventional chemicals for the regeneration of synthesized materials showed that regeneration in this study is cost effective as regeneration has been known to cost about three quarter of the total operation and maintenance of an adsorption or photocatalytic process. Application of MNP-Maph to real wastewater sampled from five different wastewater treatment plants in Eastern Cape Province for the removal of Cu2+, Zn2+ and As3+ showed that removal efficiencies of approximately 80 percent were achieved for all three metal ions upon adsorption by MNP-Maph. These therefore show that the introduction of metal loving ligand such as Maph-COOH improved the efficiency of MNP towards the removal of heavy metal ions from aqueous solution. Also, silica positively influenced the performance of magnetic titanium dioxide towards Cr(VI) reduction and separation from aqueous solution. This study therefore showed that these materials should be considered for future applications in the area of water/wastewater decontamination.
- Format
- 333 leaves
- Format
- Publisher
- University of Fort Hare
- Publisher
- Faculty of Science and Agriculture
- Language
- English
- Rights
- University of Fort Hare
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UFH Department of Chemistry
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