Harnessing low energy photons (635 nm) for the production of H2O2 using upconversion nanohybrid photocatalysts

Hyoung Il Kim, Oh Seok Kwon, Sujeong Kim, Wonyong Choi, Jae Hong Kim

Research output: Contribution to journalArticle

54 Citations (Scopus)

Abstract

This study demonstrates, for the first time in literature, in situ photocatalytic synthesis of hydrogen peroxide (H2O2) through sensitized triplet-triplet annihilation (TTA) upconversion (UC) of low-energy, sub-bandgap photons. The aqueous phase TTA-UC and subsequent photocatalytic oxygen reduction were achieved by a newly developed ternary nanohybrid that consists of three components: (1) a nano-scale silica core-shell structure that encapsulates TTA-UC chromophore-containing media; (2) a low-bandgap CdS photocatalyst on the surface of the silica nanocapsule; and (3) a graphene oxide nanodisk (GOND) as a co-catalyst. In this study, we employed a benchmark TTA-UC chromophore pair, palladium(ii) tetraphenyltetrabenzo-porphyrin sensitizer and 9,10-bis(phenylethynyl)anthracene acceptor, to upconvert red photons (λEx = 635 nm and 1.95 eV) to green photons (λEm = 505 nm and 2.45 eV). CdS is sensitized by upconverted green light to produce charge carriers, but not by incident red light without TTA-UC. The photogenerated electrons are efficiently transferred to a GOND to retard rapid charge recombination in CdS, which subsequently reduce dioxygen to produce H2O2 up to a 100 micromolar level per hour (or 3 mg L-1 h-1 with 0.5 g L-1 of GOND/CdS component only). Wrapping of CdS by a GOND was also found to markedly enhance the stability of CdS against photocorrosion without light shielding owing to its small size (ca. ∼80 nm) and transparency (α635nm = 1.85 g-1 dm3 cm-1).

Original languageEnglish
Pages (from-to)1063-1073
Number of pages11
JournalEnergy and Environmental Science
Volume9
Issue number3
DOIs
Publication statusPublished - 2016 Mar

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Graphite
Photocatalysts
Oxides
Graphene
Photons
oxide
Chromophores
Silicon Dioxide
energy
Energy gap
silica
Silica
Oxygen
Nanocapsules
Methyl Green
porphyrin
Anthracene
Porphyrins
palladium
Palladium

All Science Journal Classification (ASJC) codes

  • Environmental Chemistry
  • Renewable Energy, Sustainability and the Environment
  • Nuclear Energy and Engineering
  • Pollution

Cite this

Kim, Hyoung Il ; Kwon, Oh Seok ; Kim, Sujeong ; Choi, Wonyong ; Kim, Jae Hong. / Harnessing low energy photons (635 nm) for the production of H2O2 using upconversion nanohybrid photocatalysts. In: Energy and Environmental Science. 2016 ; Vol. 9, No. 3. pp. 1063-1073.
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abstract = "This study demonstrates, for the first time in literature, in situ photocatalytic synthesis of hydrogen peroxide (H2O2) through sensitized triplet-triplet annihilation (TTA) upconversion (UC) of low-energy, sub-bandgap photons. The aqueous phase TTA-UC and subsequent photocatalytic oxygen reduction were achieved by a newly developed ternary nanohybrid that consists of three components: (1) a nano-scale silica core-shell structure that encapsulates TTA-UC chromophore-containing media; (2) a low-bandgap CdS photocatalyst on the surface of the silica nanocapsule; and (3) a graphene oxide nanodisk (GOND) as a co-catalyst. In this study, we employed a benchmark TTA-UC chromophore pair, palladium(ii) tetraphenyltetrabenzo-porphyrin sensitizer and 9,10-bis(phenylethynyl)anthracene acceptor, to upconvert red photons (λEx = 635 nm and 1.95 eV) to green photons (λEm = 505 nm and 2.45 eV). CdS is sensitized by upconverted green light to produce charge carriers, but not by incident red light without TTA-UC. The photogenerated electrons are efficiently transferred to a GOND to retard rapid charge recombination in CdS, which subsequently reduce dioxygen to produce H2O2 up to a 100 micromolar level per hour (or 3 mg L-1 h-1 with 0.5 g L-1 of GOND/CdS component only). Wrapping of CdS by a GOND was also found to markedly enhance the stability of CdS against photocorrosion without light shielding owing to its small size (ca. ∼80 nm) and transparency (α635nm = 1.85 g-1 dm3 cm-1).",
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Harnessing low energy photons (635 nm) for the production of H2O2 using upconversion nanohybrid photocatalysts. / Kim, Hyoung Il; Kwon, Oh Seok; Kim, Sujeong; Choi, Wonyong; Kim, Jae Hong.

In: Energy and Environmental Science, Vol. 9, No. 3, 03.2016, p. 1063-1073.

Research output: Contribution to journalArticle

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AB - This study demonstrates, for the first time in literature, in situ photocatalytic synthesis of hydrogen peroxide (H2O2) through sensitized triplet-triplet annihilation (TTA) upconversion (UC) of low-energy, sub-bandgap photons. The aqueous phase TTA-UC and subsequent photocatalytic oxygen reduction were achieved by a newly developed ternary nanohybrid that consists of three components: (1) a nano-scale silica core-shell structure that encapsulates TTA-UC chromophore-containing media; (2) a low-bandgap CdS photocatalyst on the surface of the silica nanocapsule; and (3) a graphene oxide nanodisk (GOND) as a co-catalyst. In this study, we employed a benchmark TTA-UC chromophore pair, palladium(ii) tetraphenyltetrabenzo-porphyrin sensitizer and 9,10-bis(phenylethynyl)anthracene acceptor, to upconvert red photons (λEx = 635 nm and 1.95 eV) to green photons (λEm = 505 nm and 2.45 eV). CdS is sensitized by upconverted green light to produce charge carriers, but not by incident red light without TTA-UC. The photogenerated electrons are efficiently transferred to a GOND to retard rapid charge recombination in CdS, which subsequently reduce dioxygen to produce H2O2 up to a 100 micromolar level per hour (or 3 mg L-1 h-1 with 0.5 g L-1 of GOND/CdS component only). Wrapping of CdS by a GOND was also found to markedly enhance the stability of CdS against photocorrosion without light shielding owing to its small size (ca. ∼80 nm) and transparency (α635nm = 1.85 g-1 dm3 cm-1).

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