Deposition of CdS, CdS/ZnSe and CdS/ZnSe/ZnS shells around CdSeTe alloyed core quantum dots: effects on optical properties
- Adegoke, Oluwasesan, Nyokong, Tebello, Forbes, Patricia B C
- Authors: Adegoke, Oluwasesan , Nyokong, Tebello , Forbes, Patricia B C
- Date: 2015
- Language: English
- Type: Article
- Identifier: vital:7289 , http://hdl.handle.net/10962/d1020342
- Description: In this work, we synthesized water-soluble L-cysteine-capped alloyed CdSeTe core quantum dots (QDs) and investigated the structural and optical properties of deposition of each of CdS, CdS/ZnSe and CdS/ZnSe/ZnS shell layers. Photophysical results showed that the overcoating of a CdS shell around the alloyed CdSeTe core [quantum yield (QY) = 8.4%] resulted in effective confinement of the radiative exciton with an improved QY value of 93.5%. Subsequent deposition of a ZnSe shell around the CdSeTe/CdS surface decreased the QY value to 24.7%, but an increase in the QY value of up to 49.5% was observed when a ZnS shell was overcoated around the CdSeTe/CdS/ZnSe surface. QDs with shell layers showed improved stability relative to the core. Data obtained from time-resolved fluorescence measurements provided useful insight into variations in the photophysical properties of the QDs upon the formation of each shell layer. Our study suggests that the formation of CdSeTe/CdS core/shell QDs meets the requirements of quality QDs in terms of high photoluminescence QY and stability, hence further deposition of additional shells are not necessary in improving the optical properties of the core/shell QDs. Copyright © 2015 John Wiley & Sons, Ltd. , Original publication is available at http://dx.doi.org/10.1002/bio.3013
- Full Text: false
- Date Issued: 2015
- Authors: Adegoke, Oluwasesan , Nyokong, Tebello , Forbes, Patricia B C
- Date: 2015
- Language: English
- Type: Article
- Identifier: vital:7289 , http://hdl.handle.net/10962/d1020342
- Description: In this work, we synthesized water-soluble L-cysteine-capped alloyed CdSeTe core quantum dots (QDs) and investigated the structural and optical properties of deposition of each of CdS, CdS/ZnSe and CdS/ZnSe/ZnS shell layers. Photophysical results showed that the overcoating of a CdS shell around the alloyed CdSeTe core [quantum yield (QY) = 8.4%] resulted in effective confinement of the radiative exciton with an improved QY value of 93.5%. Subsequent deposition of a ZnSe shell around the CdSeTe/CdS surface decreased the QY value to 24.7%, but an increase in the QY value of up to 49.5% was observed when a ZnS shell was overcoated around the CdSeTe/CdS/ZnSe surface. QDs with shell layers showed improved stability relative to the core. Data obtained from time-resolved fluorescence measurements provided useful insight into variations in the photophysical properties of the QDs upon the formation of each shell layer. Our study suggests that the formation of CdSeTe/CdS core/shell QDs meets the requirements of quality QDs in terms of high photoluminescence QY and stability, hence further deposition of additional shells are not necessary in improving the optical properties of the core/shell QDs. Copyright © 2015 John Wiley & Sons, Ltd. , Original publication is available at http://dx.doi.org/10.1002/bio.3013
- Full Text: false
- Date Issued: 2015
Behavior of Palladium Nanoparticles in the Absence or Presence of Cobalt Tetraaminophthalocyanine for the Electrooxidation of Hydrazine
- Maringa, Audacity, Nyokong, Tebello
- Authors: Maringa, Audacity , Nyokong, Tebello
- Date: 2014
- Language: English
- Type: Article
- Identifier: vital:7305 , http://hdl.handle.net/10962/d1020382
- Description: We report on the electrodeposition of palladium nanoparticles (PdNPs) on a glassy carbon electrode (GCE) and onto a poly-CoTAPc-GCE (CoTAPc=cobalt tetraamino phthalocyanine) surface. The electrodes are denoted as PdNPs-GCE and PdNPs/poly-CoTAPc-GCE, respectively. PdNPs/poly-CoTAPc-GCE showed the best activity for the oxidation of hydrazine at the lowest potential of −0.28 V and with the highest currents. The results were further supported by electrochemical impedance spectroscopy (EIS) which showed that there was less resistance to charge transfer for PdNPs/poly-CoTAPc-GCE compared to PdNPs-GCE. The catalytic rate constant for hydrazine oxidation was 6.12×108 cm3 mol−1 s−1 using PdNPs/poly-CoTAPc-GCE. , Original publication is available at http://dx.doi.org/10.1002/elan.201400028
- Full Text: false
- Date Issued: 2014
- Authors: Maringa, Audacity , Nyokong, Tebello
- Date: 2014
- Language: English
- Type: Article
- Identifier: vital:7305 , http://hdl.handle.net/10962/d1020382
- Description: We report on the electrodeposition of palladium nanoparticles (PdNPs) on a glassy carbon electrode (GCE) and onto a poly-CoTAPc-GCE (CoTAPc=cobalt tetraamino phthalocyanine) surface. The electrodes are denoted as PdNPs-GCE and PdNPs/poly-CoTAPc-GCE, respectively. PdNPs/poly-CoTAPc-GCE showed the best activity for the oxidation of hydrazine at the lowest potential of −0.28 V and with the highest currents. The results were further supported by electrochemical impedance spectroscopy (EIS) which showed that there was less resistance to charge transfer for PdNPs/poly-CoTAPc-GCE compared to PdNPs-GCE. The catalytic rate constant for hydrazine oxidation was 6.12×108 cm3 mol−1 s−1 using PdNPs/poly-CoTAPc-GCE. , Original publication is available at http://dx.doi.org/10.1002/elan.201400028
- Full Text: false
- Date Issued: 2014
Development of Graphene/CdSe Quantum Dots-Co Phthalocyanine Nanocomposite for Oxygen Reduction Reaction
- Nyoni, Stephen, Nyokong, Tebello
- Authors: Nyoni, Stephen , Nyokong, Tebello
- Language: English
- Type: Article
- Identifier: vital:7300 , http://hdl.handle.net/10962/d1020368
- Description: Nanocomposites containing CdSe quantum dots, tetra(4-(4,6-diaminopyrimidin-2-ylthio) phthalocyaninatocobalt(II)) (CoPyPc) and reduced graphene nanosheets (rGNS) were devoloped and used for the modification of a glassy carbon electrode. Characterization of the nanocomposites was done by transmission electron microscopy (TEM) and X-ray diffraction (XRD) analyses. Cyclic voltammetry (CV) was used for electrochemical characterization of the prepared nanocomposite for oxygen reduction reaction. The oxygen reduction activity for rGNS/CdSe-CoPyPc nanocomposite was found to be superior over the individual nanomaterials in this study. The activity of the nanocomposite towards oxygen reduction was also tested for tolerance to methanol crossover effect using chronoamperometry (CA) and electrochemical impedance spectroscopy (EIS) studies. , Original publication is available at http://dx.doi.org/10.1002/elan.201400372
- Full Text: false
- Authors: Nyoni, Stephen , Nyokong, Tebello
- Language: English
- Type: Article
- Identifier: vital:7300 , http://hdl.handle.net/10962/d1020368
- Description: Nanocomposites containing CdSe quantum dots, tetra(4-(4,6-diaminopyrimidin-2-ylthio) phthalocyaninatocobalt(II)) (CoPyPc) and reduced graphene nanosheets (rGNS) were devoloped and used for the modification of a glassy carbon electrode. Characterization of the nanocomposites was done by transmission electron microscopy (TEM) and X-ray diffraction (XRD) analyses. Cyclic voltammetry (CV) was used for electrochemical characterization of the prepared nanocomposite for oxygen reduction reaction. The oxygen reduction activity for rGNS/CdSe-CoPyPc nanocomposite was found to be superior over the individual nanomaterials in this study. The activity of the nanocomposite towards oxygen reduction was also tested for tolerance to methanol crossover effect using chronoamperometry (CA) and electrochemical impedance spectroscopy (EIS) studies. , Original publication is available at http://dx.doi.org/10.1002/elan.201400372
- Full Text: false
Effects of Redox Mediators on the Catalytic Activity of Iron Porphyrins towards Oxygen Reduction in Acidic Media
- He, Qinggang, Wu, Gang, Liu, Ke, Khene, M Samson, Li, Qing, Mugadza, Tawanda, Deunf, Elise, Nyokong, Tebello, Chen, Shaowei W
- Authors: He, Qinggang , Wu, Gang , Liu, Ke , Khene, M Samson , Li, Qing , Mugadza, Tawanda , Deunf, Elise , Nyokong, Tebello , Chen, Shaowei W
- Language: English
- Type: Article
- Identifier: vital:7291 , http://hdl.handle.net/10962/d1020354
- Description: The effects of different redox mediators on the oxygen reduction reaction (ORR) catalyzed by an iron porphyrin complex, iron(III) meso-tetra(N-methyl-4-pyridyl)porphine chloride [FeIIITMPyP], in 0.1 M triflic acid were investigated by cyclic voltammetry (CV) and spectroelectrochemistry in conjunction with density functional theory (DFT) calculations. The formal potentials of the FeIIITMPyP catalyst and the redox mediators, as well as the half-wave potentials for the ORR, were determined by CV in the absence and presence of oxygen in acidic solutions. UV/Vis spectroscopic and spectroelectrochemical studies confirmed that only the 2,2′-azino-bis(3-ethylbenzothiazioline-6-sulfonic acid)diammonium salt (C18H24N6O6S4) showed effective interactions with FeIIITMPyP during the ORR. DFT calculations suggested strong interaction between FeIIITMPyP and the C18H24N6O6S4 redox mediator. The redox mediator caused lengthening of the dioxygen iron bond, which thus suggested easier dioxygen reduction. Consistent results were observed in electrochemical impedance spectroscopic measurements for which the electron-transfer kinetics were also evaluated. , Original publication is available at http://dx.doi.org/10.1002/celc.201402054
- Full Text: false
- Authors: He, Qinggang , Wu, Gang , Liu, Ke , Khene, M Samson , Li, Qing , Mugadza, Tawanda , Deunf, Elise , Nyokong, Tebello , Chen, Shaowei W
- Language: English
- Type: Article
- Identifier: vital:7291 , http://hdl.handle.net/10962/d1020354
- Description: The effects of different redox mediators on the oxygen reduction reaction (ORR) catalyzed by an iron porphyrin complex, iron(III) meso-tetra(N-methyl-4-pyridyl)porphine chloride [FeIIITMPyP], in 0.1 M triflic acid were investigated by cyclic voltammetry (CV) and spectroelectrochemistry in conjunction with density functional theory (DFT) calculations. The formal potentials of the FeIIITMPyP catalyst and the redox mediators, as well as the half-wave potentials for the ORR, were determined by CV in the absence and presence of oxygen in acidic solutions. UV/Vis spectroscopic and spectroelectrochemical studies confirmed that only the 2,2′-azino-bis(3-ethylbenzothiazioline-6-sulfonic acid)diammonium salt (C18H24N6O6S4) showed effective interactions with FeIIITMPyP during the ORR. DFT calculations suggested strong interaction between FeIIITMPyP and the C18H24N6O6S4 redox mediator. The redox mediator caused lengthening of the dioxygen iron bond, which thus suggested easier dioxygen reduction. Consistent results were observed in electrochemical impedance spectroscopic measurements for which the electron-transfer kinetics were also evaluated. , Original publication is available at http://dx.doi.org/10.1002/celc.201402054
- Full Text: false
Electrode Modification Using Alkynyl Substituted Fe(II) Phthalocyanine via Electrografting and Click Chemistry for Electrocatalysis
- Nxele, Siphesihle R, Mashazi, Philani N, Nyokong, Tebello
- Authors: Nxele, Siphesihle R , Mashazi, Philani N , Nyokong, Tebello
- Language: English
- Type: Article
- Identifier: vital:7284 , http://hdl.handle.net/10962/d1020329
- Description: In this work, tetrakis(5-hexyn-oxy)Fe(II) phthalocyanine was synthesised in order to perform a click reaction between the terminal alkyne groups and an azide group on a glassy carbon electrode (GCE) surface. An azide group was formed on the electrode surface following electrografting using 4-azidobenzene diazonium tetrafluoroborate by electrochemical reduction. The Cu(I) catalyzed alkyne-azide Huisgen cycloaddition reaction was then employed in order to react the terminal alkyne groups on the phthalocyanine with the azide groups on the GCE surface. The modified electrode was employed to catalyse the oxidation of hydrazine. The electrode showed good electrocatalytic ability towards the detection of hydrazine with a sensitivity of 15.38 µA mM−1 and a limit of detection of 1.09 µM. , Original publication is available at http://dx.doi.org/10.1002/elan.201500212
- Full Text: false
- Authors: Nxele, Siphesihle R , Mashazi, Philani N , Nyokong, Tebello
- Language: English
- Type: Article
- Identifier: vital:7284 , http://hdl.handle.net/10962/d1020329
- Description: In this work, tetrakis(5-hexyn-oxy)Fe(II) phthalocyanine was synthesised in order to perform a click reaction between the terminal alkyne groups and an azide group on a glassy carbon electrode (GCE) surface. An azide group was formed on the electrode surface following electrografting using 4-azidobenzene diazonium tetrafluoroborate by electrochemical reduction. The Cu(I) catalyzed alkyne-azide Huisgen cycloaddition reaction was then employed in order to react the terminal alkyne groups on the phthalocyanine with the azide groups on the GCE surface. The modified electrode was employed to catalyse the oxidation of hydrazine. The electrode showed good electrocatalytic ability towards the detection of hydrazine with a sensitivity of 15.38 µA mM−1 and a limit of detection of 1.09 µM. , Original publication is available at http://dx.doi.org/10.1002/elan.201500212
- Full Text: false
Iodine-Doped Cobalt Phthalocyanine Supported on Multiwalled Carbon Nanotubes for Electrocatalysis of Oxygen Reduction Reaction
- Nyoni, Stephen, Mashazi, Philani N, Nyokong, Tebello
- Authors: Nyoni, Stephen , Mashazi, Philani N , Nyokong, Tebello
- Language: English
- Type: Article
- Identifier: vital:7242 , http://hdl.handle.net/10962/d1020246
- Description: 4-(4,6-Diaminopyrimidin-2-ylthio) phthalocyaninatocobalt(II) (CoPyPc) was iodine doped, and its electrocatalytic properties explored. Physical characterization techniques such as UV-vis, X-ray photoelectron, electron paramagnetic resonance and infra-red spectroscopy were used. Cyclic voltammetry, electrochemical impedance spectroscopy and rotating disk electrode were used for electrochemical characterization of electrodes modified with the prepared phthalocyanine and its nanocomposites. The electrocatalytic effect of a new iodine-doped cobalt phthalocyanine derivative supported on multiwalled carbon nanotubes was then investigated towards oxygen reduction reaction. The electrocatalytic activity of the iodine-doped cobalt phthalocyanine was found to be superior in terms of current over the undoped phthalocyanine nanocomposite. , Original publication is available at http://dx.doi.org/10.1002/elan.201400499
- Full Text: false
- Authors: Nyoni, Stephen , Mashazi, Philani N , Nyokong, Tebello
- Language: English
- Type: Article
- Identifier: vital:7242 , http://hdl.handle.net/10962/d1020246
- Description: 4-(4,6-Diaminopyrimidin-2-ylthio) phthalocyaninatocobalt(II) (CoPyPc) was iodine doped, and its electrocatalytic properties explored. Physical characterization techniques such as UV-vis, X-ray photoelectron, electron paramagnetic resonance and infra-red spectroscopy were used. Cyclic voltammetry, electrochemical impedance spectroscopy and rotating disk electrode were used for electrochemical characterization of electrodes modified with the prepared phthalocyanine and its nanocomposites. The electrocatalytic effect of a new iodine-doped cobalt phthalocyanine derivative supported on multiwalled carbon nanotubes was then investigated towards oxygen reduction reaction. The electrocatalytic activity of the iodine-doped cobalt phthalocyanine was found to be superior in terms of current over the undoped phthalocyanine nanocomposite. , Original publication is available at http://dx.doi.org/10.1002/elan.201400499
- Full Text: false
Polyamide nanofiber membranes functionalized with zinc phthalocyanines
- Goethals, Annelies, Mugadza, Tawanda, Arslanoglu, Yasin, Zugle, Ruphino, Antunes, Edith M, Hulle, Stijn W H Van, Nyokong, Tebello, Clerck, Karen De
- Authors: Goethals, Annelies , Mugadza, Tawanda , Arslanoglu, Yasin , Zugle, Ruphino , Antunes, Edith M , Hulle, Stijn W H Van , Nyokong, Tebello , Clerck, Karen De
- Language: English
- Type: Article
- Identifier: vital:7313 , http://hdl.handle.net/10962/d1020539
- Description: Electrospinning is an efficient method for the production of polyamide nanofiber membranes that are suitable for water filtration. Previous studies have shown that nanofiber membranes have high clean water permeability. The pathogen removal efficiency can be improved by functionalization with (organic) biocides. However, these membranes, like other membranes, are vulnerable to fouling which reduces the filtration efficiency. Therefore the present article investigates the potential of zinc phthalocyanines, which can produce singlet oxygen in the presence of visible light, as a functionalizing agent. The polyamide nanofiber membranes were functionalized with phthalocyanines using both a pre-functionalizing and post-functionalizing method. Only the post-functionalization method shows to result in nanofiber membranes capable of producing singlet oxygen. After 30 min 45% of 1,2-diphenylisobenzofuran (DPBF), used as an oxygen quencher, was removed by reaction with singlet oxygen. This resulted in a removal rate of 0.33 mol DBPF mol−1Zn min−1. During short term leaching tests, phthalocyanines could not be detected. , Original publication is available at http://dx.doi.org/10.1002/app.40486
- Full Text: false
- Authors: Goethals, Annelies , Mugadza, Tawanda , Arslanoglu, Yasin , Zugle, Ruphino , Antunes, Edith M , Hulle, Stijn W H Van , Nyokong, Tebello , Clerck, Karen De
- Language: English
- Type: Article
- Identifier: vital:7313 , http://hdl.handle.net/10962/d1020539
- Description: Electrospinning is an efficient method for the production of polyamide nanofiber membranes that are suitable for water filtration. Previous studies have shown that nanofiber membranes have high clean water permeability. The pathogen removal efficiency can be improved by functionalization with (organic) biocides. However, these membranes, like other membranes, are vulnerable to fouling which reduces the filtration efficiency. Therefore the present article investigates the potential of zinc phthalocyanines, which can produce singlet oxygen in the presence of visible light, as a functionalizing agent. The polyamide nanofiber membranes were functionalized with phthalocyanines using both a pre-functionalizing and post-functionalizing method. Only the post-functionalization method shows to result in nanofiber membranes capable of producing singlet oxygen. After 30 min 45% of 1,2-diphenylisobenzofuran (DPBF), used as an oxygen quencher, was removed by reaction with singlet oxygen. This resulted in a removal rate of 0.33 mol DBPF mol−1Zn min−1. During short term leaching tests, phthalocyanines could not be detected. , Original publication is available at http://dx.doi.org/10.1002/app.40486
- Full Text: false
Ultrafast Photodynamics of the Indoline Dye D149 Adsorbed to Porous ZnO in Dye-Sensitized Solar Cells
- Rohwer, Egmont, Richter, Christoph, Heming, Nadine, Strauch, Kerstin, Litwinski, Christian, Nyokong, Tebello, Schlettwein, Derck, Schwoerer, Heinrich
- Authors: Rohwer, Egmont , Richter, Christoph , Heming, Nadine , Strauch, Kerstin , Litwinski, Christian , Nyokong, Tebello , Schlettwein, Derck , Schwoerer, Heinrich
- Language: English
- Type: Article
- Identifier: vital:7326 , http://hdl.handle.net/10962/d1020576
- Description: We investigate the ultrafast dynamics of the photoinduced electron transfer between surface-adsorbed indoline D149 dye and porous ZnO as used in the working electrodes of dye-sensitized solar cells. Transient absorption spectroscopy was conducted on the dye in solution, on solid state samples and for the latter in contact to a I−/I3− redox electrolyte typical for dye-sensitized solar cells to elucidate the effect of each component in the observed dynamics. D149 in a solution of 1:1 acetonitrile and tert-butyl alcohol shows excited-state lifetimes of 300±50 ps. This signature is severely quenched when D149 is adsorbed to ZnO, with the fastest component of the decay trace measured at 150±20 fs due to the charge-transfer mechanism. Absorption bands of the oxidized dye molecule were investigated to determine regeneration times which are in excess of 1 ns. The addition of the redox electrolyte to the system results in faster regeneration times, of the order of 1 ns. , Original publication is available at http://dx.doi.org/10.1002/cphc.201200715
- Full Text: false
- Authors: Rohwer, Egmont , Richter, Christoph , Heming, Nadine , Strauch, Kerstin , Litwinski, Christian , Nyokong, Tebello , Schlettwein, Derck , Schwoerer, Heinrich
- Language: English
- Type: Article
- Identifier: vital:7326 , http://hdl.handle.net/10962/d1020576
- Description: We investigate the ultrafast dynamics of the photoinduced electron transfer between surface-adsorbed indoline D149 dye and porous ZnO as used in the working electrodes of dye-sensitized solar cells. Transient absorption spectroscopy was conducted on the dye in solution, on solid state samples and for the latter in contact to a I−/I3− redox electrolyte typical for dye-sensitized solar cells to elucidate the effect of each component in the observed dynamics. D149 in a solution of 1:1 acetonitrile and tert-butyl alcohol shows excited-state lifetimes of 300±50 ps. This signature is severely quenched when D149 is adsorbed to ZnO, with the fastest component of the decay trace measured at 150±20 fs due to the charge-transfer mechanism. Absorption bands of the oxidized dye molecule were investigated to determine regeneration times which are in excess of 1 ns. The addition of the redox electrolyte to the system results in faster regeneration times, of the order of 1 ns. , Original publication is available at http://dx.doi.org/10.1002/cphc.201200715
- Full Text: false
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