<p>Self-reducing phosphors have attracted significant attention due to their avoidance of hazardous gases (H<sub>2</sub>/CO/N<sub>2</sub>), offering safer and more economical alternatives. This work reveals oxygen vacancy defect-induced Ce<sup>3+</sup> self-reduction behavior in garnet structure. The Ca<sub>2</sub>Gd<sub>1−<i>x</i></sub>Zr<sub>2</sub>Al<sub>3</sub>O<sub>12</sub>:Ce<sup>3+</sup> cyan phosphors were successfully synthesized via conventional high-temperature solid-state reaction in ambient atmosphere. Photoluminescence (PL) spectra revealed a strong emission centered at 490&#xa0;nm, aligning well with the cyan component required in WLEDs. The relatively short fluorescence lifetime further implies the potential of CGZA:Ce<sup>3+/4+</sup> phosphors for high-speed visible light communication (VLC). By combining electron paramagnetic resonance (EPR) spectroscopy with density functional theory (DFT) calculations, the self-reduction behavior of Ce<sup>4+</sup> to Ce<sup>3+</sup> in the garnet structure was elucidated. The results suggest that oxygen vacancies play a critical role in facilitating the reduction process. DFT calculations revealed that Ce doping significantly lowers the formation energy of oxygen vacancies, thereby promoting self-reduction. These findings provide valuable insights into the design of novel self-reducing Ce<sup>3+</sup>-based phosphors for advanced lighting and optical communication applications.</p> Graphical abstract <p></p>

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Oxygen vacancy-induced cerium self-reduction in cyan-emitting phosphors for high-quality white lighting and visible light communication applications

  • Yu-Qi Cai,
  • Chun-Yu Zuo,
  • Wei-Ling Yang,
  • Xiao-Qing Pei,
  • Yi-Feng Zhu,
  • Shuai Yang,
  • Ying-Chao Li,
  • Xin Zhao,
  • Zhuang Liu,
  • Chun Li

摘要

Self-reducing phosphors have attracted significant attention due to their avoidance of hazardous gases (H2/CO/N2), offering safer and more economical alternatives. This work reveals oxygen vacancy defect-induced Ce3+ self-reduction behavior in garnet structure. The Ca2Gd1−xZr2Al3O12:Ce3+ cyan phosphors were successfully synthesized via conventional high-temperature solid-state reaction in ambient atmosphere. Photoluminescence (PL) spectra revealed a strong emission centered at 490 nm, aligning well with the cyan component required in WLEDs. The relatively short fluorescence lifetime further implies the potential of CGZA:Ce3+/4+ phosphors for high-speed visible light communication (VLC). By combining electron paramagnetic resonance (EPR) spectroscopy with density functional theory (DFT) calculations, the self-reduction behavior of Ce4+ to Ce3+ in the garnet structure was elucidated. The results suggest that oxygen vacancies play a critical role in facilitating the reduction process. DFT calculations revealed that Ce doping significantly lowers the formation energy of oxygen vacancies, thereby promoting self-reduction. These findings provide valuable insights into the design of novel self-reducing Ce3+-based phosphors for advanced lighting and optical communication applications.

Graphical abstract