Plasmon and Upconversion Mediated Broadband Spectral Response in TiO2 Inverse Opal Photocatalysts for Enhanced Photoelectrochemical Water Splitting

Ramireddy Boppella, Filipe Marques Mota, Ju Won Lim, Saji Thomas Kochuveedu, Sunghyun Ahn, Jiseok Lee, Daisuke Kawaguchi, Keiji Tanaka, Dong Ha Kim

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Harvesting low-energy photons by strategically exploiting the photocatalytic properties of plasmonic and upconversion nanocomponents is a promising route to improve solar energy utilization. Herein, a rationally designed 3D composite photoanode integrating NIR-responsive upconversion nanocrystals (UCNs) and visible-responsive plasmonic Au nanoparticles (NPs) into 3D TiO2 inverse opal nanostructures (Au/UCN/TiO2) has been shown to extend the solar energy utilization in the UV-vis-NIR range. The NIR-responsive properties of NaYF4:Yb3+-based UCNs doped with Er3+ or Tm3+ ions, and the effect of an alternating sequential introduction of UCN and Au, have been assessed. With an extended overlap between the emission of Er-UCN and the characteristic SPR band of Au, our ternary Au/Er-UCN/TiO2 hybrid nanostructure unveiled a notable 10-fold improvement in photocurrent density under UV-vis-NIR illumination compared with a pristine TiO2 reference. The Au incorporation was confirmed to play a key role in enhancing the efficiency of light harvesting and to synergistically facilitate the energy transfer from UCNs to TiO2. This work further dissected plausible mechanistic pathways combining collected photoelectrocatalytic results, with electrochemical impedance measurements and transient absorption spectroscopic measurements. The synthesis and catalytic performance of our Au/UCN/TiO2 and the underlying mechanism here proposed are expected to reflect extended applicability in analogous applications for efficient solar-to-energy sustainable platforms.

Original languageEnglish
Pages (from-to)3780-3790
Number of pages11
JournalACS Applied Energy Materials
Volume2
Issue number5
DOIs
Publication statusPublished - May 28 2019

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Photocatalysts
Nanocrystals
Water
Solar energy
Nanostructures
Energy utilization
Photocurrents
Energy transfer
Photons
Lighting
Ions
Nanoparticles
Composite materials

All Science Journal Classification (ASJC) codes

  • Energy Engineering and Power Technology
  • Chemical Engineering (miscellaneous)
  • Electrochemistry
  • Materials Chemistry
  • Electrical and Electronic Engineering

Cite this

Plasmon and Upconversion Mediated Broadband Spectral Response in TiO2 Inverse Opal Photocatalysts for Enhanced Photoelectrochemical Water Splitting. / Boppella, Ramireddy; Marques Mota, Filipe; Lim, Ju Won; Kochuveedu, Saji Thomas; Ahn, Sunghyun; Lee, Jiseok; Kawaguchi, Daisuke; Tanaka, Keiji; Kim, Dong Ha.

In: ACS Applied Energy Materials, Vol. 2, No. 5, 28.05.2019, p. 3780-3790.

Research output: Contribution to journalArticle

Boppella, Ramireddy ; Marques Mota, Filipe ; Lim, Ju Won ; Kochuveedu, Saji Thomas ; Ahn, Sunghyun ; Lee, Jiseok ; Kawaguchi, Daisuke ; Tanaka, Keiji ; Kim, Dong Ha. / Plasmon and Upconversion Mediated Broadband Spectral Response in TiO2 Inverse Opal Photocatalysts for Enhanced Photoelectrochemical Water Splitting. In: ACS Applied Energy Materials. 2019 ; Vol. 2, No. 5. pp. 3780-3790.
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