Application of graphene quantum dots functionalized with thymine and thymine-appended zinc phthalocyanine as novel photoluminescent nanoprobes
- Achadu, Ojodomo John, Nyokong, Tebello
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188508 , vital:44760 , xlink:href="https://doi.org/10.1039/C6NJ03285K"
- Description: Graphene quantum dots (GQDs) and zinc phthalocyanine (ZnPc) were separately modified with thymine to obtain thymine-functionalized GQDs (T-GQDs) and ZnPc (T-ZnPc). T-GQDs and nanoconjugates of T-ZnPc with pristine GQDs (represented as pristine GQDs–T-ZnPc) or T-GQDs (represented as T-GQDs–T-ZnPc) were employed as fluorescent probes for the detection of mercury(II) ions (Hg2+). The as-synthesized T-GQDs alone demonstrated a highly sensitive and selective fluorescence “turn-OFF” process for Hg2+ detection due to the specific interaction between the thymine functionality on the T-GQDs with Hg2+. On the other hand, the fluorescence of pristine GQDs and T-GQDs was quenched (“turn-OFF”) upon coordination with T-ZnPc. However, the fluorescence emission was selectively restored (“turn-ON” process) in the presence of Hg2+ resulting in the sensitive detection of Hg2+ in the nanomolar concentration range (limit of detection = 0.05 nM, for the pristine GQDs–T-ZnPc probe). The probe containing pristine GQDs and the T-ZnPc complex demonstrated a higher specific and sensitive recognition of Hg2+ as compared to the T-GQDs alone or T-GQDs–T-ZnPc probes which are ascribed to the fluorescence “turn-ON” process of the former. Screening of different metal ions and counter ions proved that the probes are specifically suited for Hg2+ detection.
- Full Text:
- Date Issued: 2017
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188508 , vital:44760 , xlink:href="https://doi.org/10.1039/C6NJ03285K"
- Description: Graphene quantum dots (GQDs) and zinc phthalocyanine (ZnPc) were separately modified with thymine to obtain thymine-functionalized GQDs (T-GQDs) and ZnPc (T-ZnPc). T-GQDs and nanoconjugates of T-ZnPc with pristine GQDs (represented as pristine GQDs–T-ZnPc) or T-GQDs (represented as T-GQDs–T-ZnPc) were employed as fluorescent probes for the detection of mercury(II) ions (Hg2+). The as-synthesized T-GQDs alone demonstrated a highly sensitive and selective fluorescence “turn-OFF” process for Hg2+ detection due to the specific interaction between the thymine functionality on the T-GQDs with Hg2+. On the other hand, the fluorescence of pristine GQDs and T-GQDs was quenched (“turn-OFF”) upon coordination with T-ZnPc. However, the fluorescence emission was selectively restored (“turn-ON” process) in the presence of Hg2+ resulting in the sensitive detection of Hg2+ in the nanomolar concentration range (limit of detection = 0.05 nM, for the pristine GQDs–T-ZnPc probe). The probe containing pristine GQDs and the T-ZnPc complex demonstrated a higher specific and sensitive recognition of Hg2+ as compared to the T-GQDs alone or T-GQDs–T-ZnPc probes which are ascribed to the fluorescence “turn-ON” process of the former. Screening of different metal ions and counter ions proved that the probes are specifically suited for Hg2+ detection.
- Full Text:
- Date Issued: 2017
Characterization and physicochemical studies of the conjugates of graphene quantum dots with differently charged zinc phthalocyanines
- Matshitse, Refilwe, Sekhosana, Kutloana E, Achadu, Ojodomo John, Nyokong, Tebello
- Authors: Matshitse, Refilwe , Sekhosana, Kutloana E , Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/189227 , vital:44829 , xlink:href="https://doi.org/10.1080/00958972.2017.1387652"
- Description: Unsubstituted zinc phthalocyanine (ZnPc), 2,9,16,23-tetrakis[4-(N-methylpyridyloxy)]-phthalocyanine (ZnTPPcQ) and Zn tetrasulfo phthalocyanine (ZnTSPc) were non-covalently (electrostatic and/or π–π interaction) attached to graphene quantum dots (GQDs) to form GQDs-Pc nanoconjugates. Relative to Pcs alone, the presence of GQDs improved the triplet quantum yields with the following values: GQDs-ZnPc (0.73), GQDs-ZnTPPcQ (0.76) and GQDs-ZnTSPc (0.67). Respective Förster resonance energy transfer (FRET) efficiencies were calculated to be 0.81, 0.80 and 0.28. However, singlet oxygen generating abilities of the as-synthesized nanoconjugates were relatively low due to the screening effect of GQDs and quenching in water. This study shows that, the type of Pc, loading and solvent used are among the vital properties to consider when constructing GQD-nanoconjugate systems with optimal triplet quantum yield properties and investigation of their physicochemical properties.
- Full Text:
- Date Issued: 2017
- Authors: Matshitse, Refilwe , Sekhosana, Kutloana E , Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/189227 , vital:44829 , xlink:href="https://doi.org/10.1080/00958972.2017.1387652"
- Description: Unsubstituted zinc phthalocyanine (ZnPc), 2,9,16,23-tetrakis[4-(N-methylpyridyloxy)]-phthalocyanine (ZnTPPcQ) and Zn tetrasulfo phthalocyanine (ZnTSPc) were non-covalently (electrostatic and/or π–π interaction) attached to graphene quantum dots (GQDs) to form GQDs-Pc nanoconjugates. Relative to Pcs alone, the presence of GQDs improved the triplet quantum yields with the following values: GQDs-ZnPc (0.73), GQDs-ZnTPPcQ (0.76) and GQDs-ZnTSPc (0.67). Respective Förster resonance energy transfer (FRET) efficiencies were calculated to be 0.81, 0.80 and 0.28. However, singlet oxygen generating abilities of the as-synthesized nanoconjugates were relatively low due to the screening effect of GQDs and quenching in water. This study shows that, the type of Pc, loading and solvent used are among the vital properties to consider when constructing GQD-nanoconjugate systems with optimal triplet quantum yield properties and investigation of their physicochemical properties.
- Full Text:
- Date Issued: 2017
Effects of substituents on the electrocatalytic activity of cobalt phthalocyanines when conjugated to graphene quantum dots
- Centane, Sixolile, Achadu, Ojodomo John, Nyokong, Tebello
- Authors: Centane, Sixolile , Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188237 , vital:44737 , xlink:href="https://doi.org/10.1002/elan.201700252"
- Description: We report on the π–π interactions between graphene quantum dots (GQDs) and the following cobalt phthalocyanine derivatives: cobalt monocarboxyphenoxy phthalocyanine (complex 1), cobalt tetracarboxyphenoxyphthalocyanine (complex 2), and cobalt tetraaminophenoxy phthalocyanine (complex 3). The conjugates (conj) with GQDs are represented as 1@GQDs(conj), 2@GQDs(conj) and 3@GQDs(conj), respectively. The resulting phthalocyanine/GQDs conjugates were adsorbed on containing a glassy carbon electrode (GCE) using the drop and dry method. We explore the electrochemical properties of phthalocyanines functionalized with both electron withdrawing groups and electron donating groups when non-covalently linked to the π-electron rich graphene quantum dots. GCE/3, GCE/2@GQDs(conj) and GCE/1@GQDs(conj) had the lowest limits of detection (LOD). Sequentially modified electrodes showed less favourable detection limits compared to the conjugates.
- Full Text:
- Date Issued: 2017
- Authors: Centane, Sixolile , Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188237 , vital:44737 , xlink:href="https://doi.org/10.1002/elan.201700252"
- Description: We report on the π–π interactions between graphene quantum dots (GQDs) and the following cobalt phthalocyanine derivatives: cobalt monocarboxyphenoxy phthalocyanine (complex 1), cobalt tetracarboxyphenoxyphthalocyanine (complex 2), and cobalt tetraaminophenoxy phthalocyanine (complex 3). The conjugates (conj) with GQDs are represented as 1@GQDs(conj), 2@GQDs(conj) and 3@GQDs(conj), respectively. The resulting phthalocyanine/GQDs conjugates were adsorbed on containing a glassy carbon electrode (GCE) using the drop and dry method. We explore the electrochemical properties of phthalocyanines functionalized with both electron withdrawing groups and electron donating groups when non-covalently linked to the π-electron rich graphene quantum dots. GCE/3, GCE/2@GQDs(conj) and GCE/1@GQDs(conj) had the lowest limits of detection (LOD). Sequentially modified electrodes showed less favourable detection limits compared to the conjugates.
- Full Text:
- Date Issued: 2017
Fluorescence behaviour of supramolecular hybrids containing graphene quantum dots and pyrene-derivatized phthalocyanines and porphyrins
- Achadu, Ojodomo John, Managa, Muthumuni, Nyokong, Tebello
- Authors: Achadu, Ojodomo John , Managa, Muthumuni , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188953 , vital:44801 , xlink:href="https://doi.org/10.1016/j.jphotochem.2016.10.029"
- Description: Novel pyrene-derivatized zinc and cobalt phthalocyanines (Pcs) and porphyrins (Ps) were immobilized on graphene quantum dots (GQDs) to form GQDs-Pcs and GQDs-Ps supramolecular hybrids via the π–π stacking interaction method. Spectroscopic evidence shows that the resultant hybrids were stable owing to the strong π–π stacking interaction between the GQDs and the respective Pcs and Ps, thus leading to the fabrication of interesting and functional supramolecular hybrids by taking advantage of the delocalized π electron systems of GQDs and the macrocycles. The conjugates showed increased fluorescence quantum yields for the Pcs/Ps, but decreased values for the GQDs in the conjugates. These novel hybrid materials could potentially be deployed for studies in both fundamental and applied perspectives due to the synergistic contributions resulting from the combination of their excellent electronic and optical properties.
- Full Text:
- Date Issued: 2017
- Authors: Achadu, Ojodomo John , Managa, Muthumuni , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188953 , vital:44801 , xlink:href="https://doi.org/10.1016/j.jphotochem.2016.10.029"
- Description: Novel pyrene-derivatized zinc and cobalt phthalocyanines (Pcs) and porphyrins (Ps) were immobilized on graphene quantum dots (GQDs) to form GQDs-Pcs and GQDs-Ps supramolecular hybrids via the π–π stacking interaction method. Spectroscopic evidence shows that the resultant hybrids were stable owing to the strong π–π stacking interaction between the GQDs and the respective Pcs and Ps, thus leading to the fabrication of interesting and functional supramolecular hybrids by taking advantage of the delocalized π electron systems of GQDs and the macrocycles. The conjugates showed increased fluorescence quantum yields for the Pcs/Ps, but decreased values for the GQDs in the conjugates. These novel hybrid materials could potentially be deployed for studies in both fundamental and applied perspectives due to the synergistic contributions resulting from the combination of their excellent electronic and optical properties.
- Full Text:
- Date Issued: 2017
Graphene quantum dots anchored onto mercaptopyridine-substituted zinc phthalocyanine-Au@ Ag nanoparticle hybrid: Application as fluorescence “off-on-off” sensor for Hg2+ and biothiols
- Achadu, Ojodomo John, Nyokong, Tebello
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188194 , vital:44731 , xlink:href="https://doi.org/10.1016/j.dyepig.2017.06.002"
- Description: Novel supramolecular hybrid containing polyethyleneimine-functionalized graphene quantum dots (PEI-GQDs) and mercaptopyridine-substituted zinc phthalocyanine (Pc)-Au@Ag nano-alloys is presented in this study. The designed hybrid was employed as a dual fluorescence nanoprobe for Hg2+ and biothiol detection in aqueous solution using PEI-GQDs as the fluorescence switching signal probe. The dual sensing platform for the analytes detection is firstly, based on the quenching (turn “OFF”) of the PEI-GQDs fluorescence upon π-π interaction or electrostatic attraction with Pc-Au@Ag conjugate. The quenched fluorescence can be switched back to the “ON” mode in the presence of Hg2+ and switched “OFF” again when biothiols are introduced to capture the Hg2+ ion via the formation of the strong metal-thiol bond (Hg-S). The “off-on-off” processes were modulated by different amounts of Hg2+ and biothiols. The nanoprobes were found to be highly stable and selective towards the target analytes in the presence of other amino acids and metal ions. Also, the probes were successfully deployed in the assay of the test analytes in spiked samples.
- Full Text:
- Date Issued: 2017
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188194 , vital:44731 , xlink:href="https://doi.org/10.1016/j.dyepig.2017.06.002"
- Description: Novel supramolecular hybrid containing polyethyleneimine-functionalized graphene quantum dots (PEI-GQDs) and mercaptopyridine-substituted zinc phthalocyanine (Pc)-Au@Ag nano-alloys is presented in this study. The designed hybrid was employed as a dual fluorescence nanoprobe for Hg2+ and biothiol detection in aqueous solution using PEI-GQDs as the fluorescence switching signal probe. The dual sensing platform for the analytes detection is firstly, based on the quenching (turn “OFF”) of the PEI-GQDs fluorescence upon π-π interaction or electrostatic attraction with Pc-Au@Ag conjugate. The quenched fluorescence can be switched back to the “ON” mode in the presence of Hg2+ and switched “OFF” again when biothiols are introduced to capture the Hg2+ ion via the formation of the strong metal-thiol bond (Hg-S). The “off-on-off” processes were modulated by different amounts of Hg2+ and biothiols. The nanoprobes were found to be highly stable and selective towards the target analytes in the presence of other amino acids and metal ions. Also, the probes were successfully deployed in the assay of the test analytes in spiked samples.
- Full Text:
- Date Issued: 2017
Graphene quantum dots coordinated to mercaptopyridine-substituted phthalocyanines: Characterization and application as fluorescence “turn ON” nanoprobes
- Achadu, Ojodomo John, Nyokong, Tebello
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188293 , vital:44742 , xlink:href="https://doi.org/10.1016/j.saa.2016.11.043"
- Description: This study reports on the design of novel nanoconjugates of graphene quantum dots (GQDs) and tetra or octa-mercaptopyridine-substituted zinc and aluminium phthalocyanines (Pcs) deployed as fluorescence “turn ON” nanoprobes. The phthalocyanines were separately adsorbed onto the planar structure of graphene quantum dots (GQDs) via π-π stacking interaction to form GQDs-mercaptopyridine Pcs nanoconjugates. The quaternized Pc complexes could also interact with the GQDs through electrostatic attraction due to the positive charges on the Pcs ring substituents and the negative charges on the surface of GQDs. The fluorescence emission of the GQDs was quenched upon coordination to the respective Pcs. However, the fluorescence emission was “turned ON” in the presence of Hg2 + employed as a test analyte. The mechanism of the “turn ON” of the GQDs emission in the nanoconjugates is ascribed to the strong affinity of Hg2 + to bind with the bridging sulfur on the Pcs periphery thereby disrupting the π-π stacking interaction between the GQDs and the Pcs with a consequent “turn ON” of the coordinated GQDs' fluorescence.
- Full Text:
- Date Issued: 2017
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188293 , vital:44742 , xlink:href="https://doi.org/10.1016/j.saa.2016.11.043"
- Description: This study reports on the design of novel nanoconjugates of graphene quantum dots (GQDs) and tetra or octa-mercaptopyridine-substituted zinc and aluminium phthalocyanines (Pcs) deployed as fluorescence “turn ON” nanoprobes. The phthalocyanines were separately adsorbed onto the planar structure of graphene quantum dots (GQDs) via π-π stacking interaction to form GQDs-mercaptopyridine Pcs nanoconjugates. The quaternized Pc complexes could also interact with the GQDs through electrostatic attraction due to the positive charges on the Pcs ring substituents and the negative charges on the surface of GQDs. The fluorescence emission of the GQDs was quenched upon coordination to the respective Pcs. However, the fluorescence emission was “turned ON” in the presence of Hg2 + employed as a test analyte. The mechanism of the “turn ON” of the GQDs emission in the nanoconjugates is ascribed to the strong affinity of Hg2 + to bind with the bridging sulfur on the Pcs periphery thereby disrupting the π-π stacking interaction between the GQDs and the Pcs with a consequent “turn ON” of the coordinated GQDs' fluorescence.
- Full Text:
- Date Issued: 2017
Graphene quantum dots decorated with maleimide and zinc tetramaleimido-phthalocyanine: Application in the design of “OFF-ON” fluorescence sensors for biothiols
- Achadu, Ojodomo John, Nyokong, Tebello
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188282 , vital:44741 , xlink:href="https://doi.org/10.1016/j.talanta.2017.01.031"
- Description: The fabrication of maleimide-derivatized graphene quantum dots (M-GQDs) and zinc phthalocyanine (2) as novel sensor probes for the selective detection of biothiols (cysteine, homocysteine or glutathione) through the rapid and specific Michael addition reaction between biothiols and the maleimide-derivatized probes is presented in this study. GQDs directly functionalized with maleimide units (M-GQDs) were synthesized and deployed for biothiols recognition following the principle of Michael addition. M-GQDs probe was found to be highly sensitive and selective towards biothiols detection in the nanomolar range in aqueous solution and at physiological pH (7.0). On the other hand, non-covalent interaction between pristine GQDs and novel zinc tetramaleimido-derivatized phthalocyanine resulted in the quenching of the pristine GQDs fluorescence emission which was switched back to the “ON” mode by Michael addition mechanism in the presence of biothiols. Tested relevant biomolecules did not interfere in the quantitative recognition of the biothiols. The probes showed to be highly sensitive, specific and selective for biothiols sensing in simulated real samples.
- Full Text:
- Date Issued: 2017
- Authors: Achadu, Ojodomo John , Nyokong, Tebello
- Date: 2017
- Subjects: To be catalogued
- Language: English
- Type: text , article
- Identifier: http://hdl.handle.net/10962/188282 , vital:44741 , xlink:href="https://doi.org/10.1016/j.talanta.2017.01.031"
- Description: The fabrication of maleimide-derivatized graphene quantum dots (M-GQDs) and zinc phthalocyanine (2) as novel sensor probes for the selective detection of biothiols (cysteine, homocysteine or glutathione) through the rapid and specific Michael addition reaction between biothiols and the maleimide-derivatized probes is presented in this study. GQDs directly functionalized with maleimide units (M-GQDs) were synthesized and deployed for biothiols recognition following the principle of Michael addition. M-GQDs probe was found to be highly sensitive and selective towards biothiols detection in the nanomolar range in aqueous solution and at physiological pH (7.0). On the other hand, non-covalent interaction between pristine GQDs and novel zinc tetramaleimido-derivatized phthalocyanine resulted in the quenching of the pristine GQDs fluorescence emission which was switched back to the “ON” mode by Michael addition mechanism in the presence of biothiols. Tested relevant biomolecules did not interfere in the quantitative recognition of the biothiols. The probes showed to be highly sensitive, specific and selective for biothiols sensing in simulated real samples.
- Full Text:
- Date Issued: 2017
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