One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes

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Authors

  • Pawan Pathak
  • Mateusz Podzorski
  • Detlef Bahnemann
  • Vaidyanathan Ravi Subramanian

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Original languageEnglish
Pages (from-to)13659-13668
Number of pages10
JournalThe Journal of Physical Chemistry C
Volume122
Issue number25
Early online date6 Apr 2018
Publication statusPublished - 28 Jun 2018

Abstract

Lead sulfide quantum dot nanocrystal (QDNC) sensitized TiO 2 nanotubes have been fabricated using a simple, wet chemical method that is both time- and cost-effective. A single precursor source containing both Pb and S has been employed, with oleylamine as a linker molecule to synthesize the PbS under an ambient pressure based approach. This approach serves to assemble the QDNCs on a TiO 2 nanotube surface. Surface characterization was performed using electron microscopy, X-ray diffraction, and elemental analysis, indicating the formation of PbS quantum dots along the nanotube walls and intertubular spacing. The optoelectronic, photoelectrochemical, and photocatalytic properties of the composite heterostructure have been characterized using absorbance spectroscopy, electrochemical studies (including efficiency measurements), and methylene blue conversion as a probe. A 24-fold increase in the photocurrent of TiO 2-PbS heterostructure over bare TiO 2 nanotube has been observed. Electrochemical impedance measurements of the TiO 2 nanotube sample indicate donor density of ∼4.5 × 10 19 cm -3 while TiO 2/PbS heterostructure shows an n-n photoactive heterojunction with a donor density of ∼2.3 × 10 20 cm -3. A 12% increase in photocatalytic activity and theoretical estimates suggesting almost 40-fold enhancement toward value-added product synthesis with PbS inclusion are presented.

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One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes. / Pathak, Pawan; Podzorski, Mateusz; Bahnemann, Detlef et al.
In: The Journal of Physical Chemistry C, Vol. 122, No. 25, 28.06.2018, p. 13659-13668.

Research output: Contribution to journalArticleResearchpeer review

Pathak, P, Podzorski, M, Bahnemann, D & Subramanian, VR 2018, 'One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes', The Journal of Physical Chemistry C, vol. 122, no. 25, pp. 13659-13668. https://doi.org/10.1021/acs.jpcc.8b00120
Pathak, P., Podzorski, M., Bahnemann, D., & Subramanian, V. R. (2018). One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes. The Journal of Physical Chemistry C, 122(25), 13659-13668. https://doi.org/10.1021/acs.jpcc.8b00120
Pathak P, Podzorski M, Bahnemann D, Subramanian VR. One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes. The Journal of Physical Chemistry C. 2018 Jun 28;122(25):13659-13668. Epub 2018 Apr 6. doi: 10.1021/acs.jpcc.8b00120
Pathak, Pawan ; Podzorski, Mateusz ; Bahnemann, Detlef et al. / One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes. In: The Journal of Physical Chemistry C. 2018 ; Vol. 122, No. 25. pp. 13659-13668.
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title = "One-Pot Fabrication of High Coverage PbS Quantum Dot Nanocrystal-Sensitized Titania Nanotubes for Photoelectrochemical Processes",
abstract = "Lead sulfide quantum dot nanocrystal (QDNC) sensitized TiO 2 nanotubes have been fabricated using a simple, wet chemical method that is both time- and cost-effective. A single precursor source containing both Pb and S has been employed, with oleylamine as a linker molecule to synthesize the PbS under an ambient pressure based approach. This approach serves to assemble the QDNCs on a TiO 2 nanotube surface. Surface characterization was performed using electron microscopy, X-ray diffraction, and elemental analysis, indicating the formation of PbS quantum dots along the nanotube walls and intertubular spacing. The optoelectronic, photoelectrochemical, and photocatalytic properties of the composite heterostructure have been characterized using absorbance spectroscopy, electrochemical studies (including efficiency measurements), and methylene blue conversion as a probe. A 24-fold increase in the photocurrent of TiO 2-PbS heterostructure over bare TiO 2 nanotube has been observed. Electrochemical impedance measurements of the TiO 2 nanotube sample indicate donor density of ∼4.5 × 10 19 cm -3 while TiO 2/PbS heterostructure shows an n-n photoactive heterojunction with a donor density of ∼2.3 × 10 20 cm -3. A 12% increase in photocatalytic activity and theoretical estimates suggesting almost 40-fold enhancement toward value-added product synthesis with PbS inclusion are presented. ",
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note = "Funding information: RSV gratefully acknowledges NSF funding (CBET 1337050) for partially supporting the initial part of this project. RSV would like to thank the the Alexander von Humboldt Foundation for supporting him to collaborate with Prof. Bahnemann{\textquoteright}s Laboratory. RSV thanks Dr. Mo Ahmedian for HRTEM studies. He also acknowledges NSF - EPSCOR UG support for MP.",
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N1 - Funding information: RSV gratefully acknowledges NSF funding (CBET 1337050) for partially supporting the initial part of this project. RSV would like to thank the the Alexander von Humboldt Foundation for supporting him to collaborate with Prof. Bahnemann’s Laboratory. RSV thanks Dr. Mo Ahmedian for HRTEM studies. He also acknowledges NSF - EPSCOR UG support for MP.

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N2 - Lead sulfide quantum dot nanocrystal (QDNC) sensitized TiO 2 nanotubes have been fabricated using a simple, wet chemical method that is both time- and cost-effective. A single precursor source containing both Pb and S has been employed, with oleylamine as a linker molecule to synthesize the PbS under an ambient pressure based approach. This approach serves to assemble the QDNCs on a TiO 2 nanotube surface. Surface characterization was performed using electron microscopy, X-ray diffraction, and elemental analysis, indicating the formation of PbS quantum dots along the nanotube walls and intertubular spacing. The optoelectronic, photoelectrochemical, and photocatalytic properties of the composite heterostructure have been characterized using absorbance spectroscopy, electrochemical studies (including efficiency measurements), and methylene blue conversion as a probe. A 24-fold increase in the photocurrent of TiO 2-PbS heterostructure over bare TiO 2 nanotube has been observed. Electrochemical impedance measurements of the TiO 2 nanotube sample indicate donor density of ∼4.5 × 10 19 cm -3 while TiO 2/PbS heterostructure shows an n-n photoactive heterojunction with a donor density of ∼2.3 × 10 20 cm -3. A 12% increase in photocatalytic activity and theoretical estimates suggesting almost 40-fold enhancement toward value-added product synthesis with PbS inclusion are presented.

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