Adsorption and separation of platinum and palladium by polyamine functionalized polystyrene-based beads and nanofibers
- Fayemi, Omolola E, Ogunlaja, Adeniyi S, Kempgens, Pierre F M, Antunes, Edith M, Torto, Nelson, Nyokong, Tebello, Tshentu, Zenixole R
- Authors: Fayemi, Omolola E , Ogunlaja, Adeniyi S , Kempgens, Pierre F M , Antunes, Edith M , Torto, Nelson , Nyokong, Tebello , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241694 , vital:50961 , xlink:href="https://doi.org/10.1016/j.mineng.2013.06.006"
- Description: Adsorption and separation of platinum and palladium chlorido species (PtCl62- and PdCl42-) on polystyrene beads as well as nanofibers functionalized with ammonium centres based on ethylenediamine (EDA), diethylenetriamine (DETA), triethylenetetramine (TETA) and tris-(2-aminoethyl)amine (TAEA) are described. The functionalized sorbent materials were characterized by microanalysis, SEM, XPS, BET and FTIR. The surface area of the functionalized fibers was in the range 69–241 m2/g while it was 73–107 m2/g for the beads. The adsorption and loading capacities of the sorption materials were investigated using both the batch and column studies at 1 M HCl concentration. The adsorption studies for both PtCl62- and PdCl42- on the different sorbent materials fit the Langmuir isotherm with R2 values >0.99. The highest loading capacity of Pt and Pd were 7.4 mg/g and 4.3 mg/g respectively for the nanofiber sorbent material based on ethylenediamine (EDA) while the beads with ethylenediamine (EDA) gave 1.0 mg/g and 0.2 mg/g for Pt and Pd respectively. Metals loaded on the sorbent materials were recovered by using 3% m/v thiourea solution as the eluting agent with quantitative desorption efficiency under the selected experimental conditions. Separation of platinum from palladium was partially achieved by selective stripping of PtCl62- with 0.5 M of NaClO4 in 1.0 M HCl while PdCl42- was eluted with 0.5 M thiourea in 1.0 M HCl. Separation of platinum from iridium and rhodium under 1 M HCl concentration was successful on triethylenetriamine (TETA)-functionalized Merrifield beads. This material (M-TETA) showed selectivity for platinum albeit the low loading capacity.
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- Authors: Fayemi, Omolola E , Ogunlaja, Adeniyi S , Kempgens, Pierre F M , Antunes, Edith M , Torto, Nelson , Nyokong, Tebello , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241694 , vital:50961 , xlink:href="https://doi.org/10.1016/j.mineng.2013.06.006"
- Description: Adsorption and separation of platinum and palladium chlorido species (PtCl62- and PdCl42-) on polystyrene beads as well as nanofibers functionalized with ammonium centres based on ethylenediamine (EDA), diethylenetriamine (DETA), triethylenetetramine (TETA) and tris-(2-aminoethyl)amine (TAEA) are described. The functionalized sorbent materials were characterized by microanalysis, SEM, XPS, BET and FTIR. The surface area of the functionalized fibers was in the range 69–241 m2/g while it was 73–107 m2/g for the beads. The adsorption and loading capacities of the sorption materials were investigated using both the batch and column studies at 1 M HCl concentration. The adsorption studies for both PtCl62- and PdCl42- on the different sorbent materials fit the Langmuir isotherm with R2 values >0.99. The highest loading capacity of Pt and Pd were 7.4 mg/g and 4.3 mg/g respectively for the nanofiber sorbent material based on ethylenediamine (EDA) while the beads with ethylenediamine (EDA) gave 1.0 mg/g and 0.2 mg/g for Pt and Pd respectively. Metals loaded on the sorbent materials were recovered by using 3% m/v thiourea solution as the eluting agent with quantitative desorption efficiency under the selected experimental conditions. Separation of platinum from palladium was partially achieved by selective stripping of PtCl62- with 0.5 M of NaClO4 in 1.0 M HCl while PdCl42- was eluted with 0.5 M thiourea in 1.0 M HCl. Separation of platinum from iridium and rhodium under 1 M HCl concentration was successful on triethylenetriamine (TETA)-functionalized Merrifield beads. This material (M-TETA) showed selectivity for platinum albeit the low loading capacity.
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Oxovanadium (IV)-containing poly (styrene-co-4′-ethenyl-2-hydroxyphenylimidazole) electrospun nanofibers for the catalytic oxidation of thioanisole
- Walmsley, Ryan S, Litwinski, Christian, Antunes, Edith M, Hlangothi, Percy, Hosten, Eric C, McCleland, Cedric, Nyokong, Tebello, Torto, Nelson, Tshentu, Zenixole R
- Authors: Walmsley, Ryan S , Litwinski, Christian , Antunes, Edith M , Hlangothi, Percy , Hosten, Eric C , McCleland, Cedric , Nyokong, Tebello , Torto, Nelson , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241665 , vital:50959 , xlink:href="https://doi.org/10.1016/j.molcata.2013.07.018"
- Description: The catalytic fibers have been fabricated by the electrospinning of a copolymer of styrene and 2-(2′-hydroxy-4′-ethenylphenyl)imidazole {p(ST-co-VPIM)} followed by a reaction with a methanolic vanadyl solution to afford the oxovanadium(IV)-containing poly(styrene-co-4′-ethenyl-2-hydroxyphenylimidazole) fibers {p(ST-co-VPIM)-VO fibers}. The relationship between polymer concentration and fiber diameter was investigated, and at high concentration (20 wt%) the fibers were quite large (average diameter of 3.8 μm) but as the concentration was reduced fibers of much lower diameter were produced (0.6 μm using 8 wt%). The BET surface area for p(ST-co-VPIM) fibers (0.6 μm diameter) was 47.9 m2 g−1 and functionalization of p(ST-co-VPIM) with vanadyl resulted in an increase in surface area to 60.7 m2 g−1 for p(ST-co-VPIM)-VO. The presence of vanadyl was confirmed by XPS and EPR. The EPR spectral analyses depicted complex speciation of vanadium within these polymer supports. These catalytic fibers were applied under batch and continuous flow conditions for the catalytic oxidation of thioanisole using hydrogen peroxide. The continuous flow method gave excellent and constant conversion throughout the 10 h period studied. The leaching of vanadium from the fiber support was 4% over the 10 h period indicating a significant stability of the material.
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- Authors: Walmsley, Ryan S , Litwinski, Christian , Antunes, Edith M , Hlangothi, Percy , Hosten, Eric C , McCleland, Cedric , Nyokong, Tebello , Torto, Nelson , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241665 , vital:50959 , xlink:href="https://doi.org/10.1016/j.molcata.2013.07.018"
- Description: The catalytic fibers have been fabricated by the electrospinning of a copolymer of styrene and 2-(2′-hydroxy-4′-ethenylphenyl)imidazole {p(ST-co-VPIM)} followed by a reaction with a methanolic vanadyl solution to afford the oxovanadium(IV)-containing poly(styrene-co-4′-ethenyl-2-hydroxyphenylimidazole) fibers {p(ST-co-VPIM)-VO fibers}. The relationship between polymer concentration and fiber diameter was investigated, and at high concentration (20 wt%) the fibers were quite large (average diameter of 3.8 μm) but as the concentration was reduced fibers of much lower diameter were produced (0.6 μm using 8 wt%). The BET surface area for p(ST-co-VPIM) fibers (0.6 μm diameter) was 47.9 m2 g−1 and functionalization of p(ST-co-VPIM) with vanadyl resulted in an increase in surface area to 60.7 m2 g−1 for p(ST-co-VPIM)-VO. The presence of vanadyl was confirmed by XPS and EPR. The EPR spectral analyses depicted complex speciation of vanadium within these polymer supports. These catalytic fibers were applied under batch and continuous flow conditions for the catalytic oxidation of thioanisole using hydrogen peroxide. The continuous flow method gave excellent and constant conversion throughout the 10 h period studied. The leaching of vanadium from the fiber support was 4% over the 10 h period indicating a significant stability of the material.
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The development of catalytic oxovanadium (IV)-containing microspheres for the oxidation of various organosulfur compounds
- Ogunlaja, Adeniyi S, Khene, Samson M, Antunes, Edith M, Nyokong, Tebello, Torto, Nelson, Tshentu, Zenixole R
- Authors: Ogunlaja, Adeniyi S , Khene, Samson M , Antunes, Edith M , Nyokong, Tebello , Torto, Nelson , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241783 , vital:50969 , xlink:href="https://doi.org/10.1016/j.apcata.2013.05.004"
- Description: The development of poly[allylSB-co-EGDMA] beads containing a tetradentate ligand was achieved via suspension polymerization. The catalyst poly[allylSB-co-EGDMA]-VO was synthesized by reacting VIVOSO4 with poly[allylSB-co-EGDMA]. XPS and EPR were used to confirm the presence of vanadium (V4+) on the beads. The synthesized catalyst (poly[allylSB-co-EGDMA]-VO) was found to have a BET surface area of 22 m2 g−1 and porosity of 135 Å, with the atomic force microscopy (AFM) showing more insight on the porous nature of the beads. Oxidation of thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) was carried out using tert-butyl hydroperoxide (t-BuOOH) as oxidant. An overall conversion of 60%, 82%, 98% and 87% was achieved for thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6 dimethyldibenzothiophene (4,6-DMDBT) respectively at higher (t-BuOOH) to substrate ratio and at a temperature of 40 °C. The efficient oxidation of the various organosulfur compounds presents potential for the possible application of this catalyst in oxidative desulfurization (ODS) of crude oil.
- Full Text:
- Authors: Ogunlaja, Adeniyi S , Khene, Samson M , Antunes, Edith M , Nyokong, Tebello , Torto, Nelson , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241783 , vital:50969 , xlink:href="https://doi.org/10.1016/j.apcata.2013.05.004"
- Description: The development of poly[allylSB-co-EGDMA] beads containing a tetradentate ligand was achieved via suspension polymerization. The catalyst poly[allylSB-co-EGDMA]-VO was synthesized by reacting VIVOSO4 with poly[allylSB-co-EGDMA]. XPS and EPR were used to confirm the presence of vanadium (V4+) on the beads. The synthesized catalyst (poly[allylSB-co-EGDMA]-VO) was found to have a BET surface area of 22 m2 g−1 and porosity of 135 Å, with the atomic force microscopy (AFM) showing more insight on the porous nature of the beads. Oxidation of thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) was carried out using tert-butyl hydroperoxide (t-BuOOH) as oxidant. An overall conversion of 60%, 82%, 98% and 87% was achieved for thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6 dimethyldibenzothiophene (4,6-DMDBT) respectively at higher (t-BuOOH) to substrate ratio and at a temperature of 40 °C. The efficient oxidation of the various organosulfur compounds presents potential for the possible application of this catalyst in oxidative desulfurization (ODS) of crude oil.
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The development of novel nickel selective amine extractants
- Okewole, Adeleye I, Antunes, Edith M, Nyokong, Tebello, Tshentu, Zenixole R
- Authors: Okewole, Adeleye I , Antunes, Edith M , Nyokong, Tebello , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241641 , vital:50957 , xlink:href="https://doi.org/10.1016/j.mineng.2013.04.019"
- Description: A chelating ion exchanger, prepared by functionalising Merrifield resin with 2,2′-pyridylimidazole, was utilized to selectively adsorb and separate nickel from other base metal ions in synthetic sulfate solutions. The sorbent material was characterized by scanning electron microscopy (SEM), microanalysis, infrared (IR), X-ray photoelectron spectroscopy (XPS) and BET surface area. The distribution ratio (D) and the sorption capacity of the microspheres toward Ni(II), Cu(II), Co(II) and Fe(II) ions was studied by using the batch and column methods, respectively. Ni(II) followed by Cu(II) showed the highest distribution ratio (D) and the highest sorption efficiency of nickel(II) ions around pH 2. The binary separation of nickel(II) from copper(II), cobalt(II) and iron(II) respectively, undertaken in a column study, through loading the metal ions at pH ≈ 2 followed by selective decomplexation, demonstrated the selectivity of the sorbent material for nickel(II). Thus, 2,2′-pyridylimidazole can be regarded as a nickel-specific extractant.
- Full Text:
- Authors: Okewole, Adeleye I , Antunes, Edith M , Nyokong, Tebello , Tshentu, Zenixole R
- Date: 2013
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/241641 , vital:50957 , xlink:href="https://doi.org/10.1016/j.mineng.2013.04.019"
- Description: A chelating ion exchanger, prepared by functionalising Merrifield resin with 2,2′-pyridylimidazole, was utilized to selectively adsorb and separate nickel from other base metal ions in synthetic sulfate solutions. The sorbent material was characterized by scanning electron microscopy (SEM), microanalysis, infrared (IR), X-ray photoelectron spectroscopy (XPS) and BET surface area. The distribution ratio (D) and the sorption capacity of the microspheres toward Ni(II), Cu(II), Co(II) and Fe(II) ions was studied by using the batch and column methods, respectively. Ni(II) followed by Cu(II) showed the highest distribution ratio (D) and the highest sorption efficiency of nickel(II) ions around pH 2. The binary separation of nickel(II) from copper(II), cobalt(II) and iron(II) respectively, undertaken in a column study, through loading the metal ions at pH ≈ 2 followed by selective decomplexation, demonstrated the selectivity of the sorbent material for nickel(II). Thus, 2,2′-pyridylimidazole can be regarded as a nickel-specific extractant.
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The development of catalytic oxovanadium(IV)-containing microspheres for the oxidation of various organosulfur compounds
- Ogunlaja, Adeniyi S, Khene, M Samson, Antunes, Edith M, Nyokong, Tebello, Torto, Nelson, Tshentu, Zenixole R
- Authors: Ogunlaja, Adeniyi S , Khene, M Samson , Antunes, Edith M , Nyokong, Tebello , Torto, Nelson , Tshentu, Zenixole R
- Language: English
- Type: Article
- Identifier: vital:7324 , http://hdl.handle.net/10962/d1020574
- Description: The development of poly[allylSB-co-EGDMA] beads containing a tetradentate ligand was achieved via suspension polymerization. The catalyst poly[allylSB-co-EGDMA]-VO was synthesized by reacting VIVOSO4 with poly[allylSB-co-EGDMA]. XPS and EPR were used to confirm the presence of vanadium (V4+) on the beads. The synthesized catalyst (poly[allylSB-co-EGDMA]-VO) was found to have a BET surface area of 22 m2 g−1 and porosity of 135 Å, with the atomic force microscopy (AFM) showing more insight on the porous nature of the beads. Oxidation of thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) was carried out using tert-butyl hydroperoxide (t-BuOOH) as oxidant. An overall conversion of 60%, 82%, 98% and 87% was achieved for thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6 dimethyldibenzothiophene (4,6-DMDBT) respectively at higher (t-BuOOH) to substrate ratio and at a temperature of 40 °C. The efficient oxidation of the various organosulfur compounds presents potential for the possible application of this catalyst in oxidative desulfurization (ODS) of crude oil. , Original publication is available at http://dx.doi.org/10.1016/j.apcata.2013.05.004
- Full Text: false
- Authors: Ogunlaja, Adeniyi S , Khene, M Samson , Antunes, Edith M , Nyokong, Tebello , Torto, Nelson , Tshentu, Zenixole R
- Language: English
- Type: Article
- Identifier: vital:7324 , http://hdl.handle.net/10962/d1020574
- Description: The development of poly[allylSB-co-EGDMA] beads containing a tetradentate ligand was achieved via suspension polymerization. The catalyst poly[allylSB-co-EGDMA]-VO was synthesized by reacting VIVOSO4 with poly[allylSB-co-EGDMA]. XPS and EPR were used to confirm the presence of vanadium (V4+) on the beads. The synthesized catalyst (poly[allylSB-co-EGDMA]-VO) was found to have a BET surface area of 22 m2 g−1 and porosity of 135 Å, with the atomic force microscopy (AFM) showing more insight on the porous nature of the beads. Oxidation of thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) was carried out using tert-butyl hydroperoxide (t-BuOOH) as oxidant. An overall conversion of 60%, 82%, 98% and 87% was achieved for thiophene (TH), benzothiophene (BT), dibenzothiophene (DBT) and 4,6 dimethyldibenzothiophene (4,6-DMDBT) respectively at higher (t-BuOOH) to substrate ratio and at a temperature of 40 °C. The efficient oxidation of the various organosulfur compounds presents potential for the possible application of this catalyst in oxidative desulfurization (ODS) of crude oil. , Original publication is available at http://dx.doi.org/10.1016/j.apcata.2013.05.004
- Full Text: false
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