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 language | English |
|---|---|
| Pages (from-to) | 3780-3790 |
| Number of pages | 11 |
| Journal | ACS Applied Energy Materials |
| Volume | 2 |
| Issue number | 5 |
| DOIs | |
| Publication status | Published - May 28 2019 |
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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 journal › Article
}
TY - JOUR
T1 - Plasmon and Upconversion Mediated Broadband Spectral Response in TiO2 Inverse Opal Photocatalysts for Enhanced Photoelectrochemical Water Splitting
AU - Boppella, Ramireddy
AU - Marques Mota, Filipe
AU - Lim, Ju Won
AU - Kochuveedu, Saji Thomas
AU - Ahn, Sunghyun
AU - Lee, Jiseok
AU - Kawaguchi, Daisuke
AU - Tanaka, Keiji
AU - Kim, Dong Ha
PY - 2019/5/28
Y1 - 2019/5/28
N2 - 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.
AB - 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.
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U2 - 10.1021/acsaem.9b00469
DO - 10.1021/acsaem.9b00469
M3 - Article
AN - SCOPUS:85065083901
VL - 2
SP - 3780
EP - 3790
JO - ACS Applied Energy Materials
JF - ACS Applied Energy Materials
SN - 2574-0962
IS - 5
ER -