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

  • 주제(키워드) surface plasmon , upconversion , broadband absorption , TiO2 inverse opal , water splitting
  • 주제(기타) Chemistry, Physical
  • 주제(기타) Energy & Fuels
  • 주제(기타) Materials Science, Multidisciplinary
  • 설명문(일반) [Boppella, Ramireddy; Mota, Filipe Marques; Lim, Ju Won; Kochuveedu, Saji Thomas; Kim, Dong Ha] Ewha Womans Univ, Dept Chem & Nano Sci, 52 Ewhayeodae Gil, Seoul 03760, South Korea; [Ahn, Sunghyun; Lee, Jiseok] Ulsan Natl Inst Sci & Technol, Sch Energy & Chem Engn, 50 UNIST Gil, Ulsan 44919, South Korea; [Kawaguchi, Daisuke; Tanaka, Keiji] Kyushu Univ, Dept Appl Chem, Fukuoka, Fukuoka 8190395, Japan; [Kawaguchi, Daisuke; Tanaka, Keiji] Kyushu Univ, Int Inst Carbon Neutral Energy Res WPI I2CNER, Fukuoka, Fukuoka 8190395, Japan
  • 등재 SCOPUS
  • 발행기관 AMER CHEMICAL SOC
  • 발행년도 2019
  • 총서유형 Journal
  • URI http://www.dcollection.net/handler/ewha/000000171994
  • 본문언어 영어
  • Published As https://dx.doi.org/10.1021/acsaem.9b00469

초록/요약

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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