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Peer-reviewedCC BY-NC 3.0Chemical Science

Selective H2O2 photosynthesis in ferroelectric photocatalyst: rare-earth 4f-state-mediated charge–spin regulation

  • Renzhi Xiong1
  • Yiyun Wang1
  • Enyi Hong1
  • Yanhe Xiao1
  • Baochang Cheng1
  • Shuijin Lei1
  1. 1School of Physics and Materials Science, Nanchang University Nanchang 330031 China
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Abstract

Solar-driven photocatalytic H2O2 synthesis is critically hampered by bulk charge recombination and spin-forbidden surface kinetics. This study proposes a rare-earth 4f-state-mediated strategy that simultaneously reconstructs the band structure and induces spin polarization. Using Aurivillius-phase Bi3TiNbO9 as a ferroelectric model system, we show that low-concentration Ce doping engenders three synergistic effects via a full-pathway charge-dynamics regulation: (i) Ce-induced lattice distortion enhances ferroelectric polarization, reinforcing the polarization electric field for directional charge separation; (ii) band-edge reconstruction reduces both carrier effective masses and exciton binding energy, accelerating exciton dissociation and carrier transport; and (iii) the unpaired 4f1 electron of Ce3+ induces spin polarization, effectively lowering the spin-related kinetic barriers for H2O2 generation. Consequently, Ce-doped Bi3TiNbO9 delivers an H2O2 production rate of 1151.7 µmol g−1 h−1 in pure water, a 6.9-fold enhancement over pristine Bi3TiNbO9. Critically, applying a 300 mT external magnetic field further boosts the rate to 1831.2 µmol g−1 h−1, providing direct evidence for spin-polarization-controlled photocatalysis. H2O2 is selectively generated through synergistic 2e− oxygen reduction reaction (ORR) and water oxidation reaction (WOR) pathways, while the competing side reactions are effectively suppressed. This work demonstrates an integrated 4f-mediated charge–spin regulation strategy that couples charge separation with spin-dependent surface reaction kinetics for efficient H2O2 photosynthesis.

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Cite

BibTeXRIS
BibTeX
@article{xiong2026selective,
  title = {{Selective H2O2 photosynthesis in ferroelectric photocatalyst: rare-earth 4f-state-mediated charge–spin regulation}},
  author = {Renzhi Xiong and Yiyun Wang and Enyi Hong and Yanhe Xiao and Baochang Cheng and Shuijin Lei},
  journal = {Chemical Science},
  year = {2026},
  month = aug,
  doi = {10.1039/d6sc04986a},
  url = {https://doi.org/10.1039/d6sc04986a},
  note = {CC BY-NC 3.0},
}
RIS
TY  - JOUR
TI  - Selective H2O2 photosynthesis in ferroelectric photocatalyst: rare-earth 4f-state-mediated charge–spin regulation
AU  - Renzhi Xiong
AU  - Yiyun Wang
AU  - Enyi Hong
AU  - Yanhe Xiao
AU  - Baochang Cheng
AU  - Shuijin Lei
PY  - 2026
DA  - 2026/08/28
JO  - Chemical Science
DO  - 10.1039/d6sc04986a
UR  - https://doi.org/10.1039/d6sc04986a
AB  - Solar-driven photocatalytic H2O2 synthesis is critically hampered by bulk charge recombination and spin-forbidden surface kinetics. This study proposes a rare-earth 4f-state-mediated strategy that simultaneously reconstructs the band structure and induces spin polarization. Using Aurivillius-phase Bi3TiNbO9 as a ferroelectric model system, we show that low-concentration Ce doping engenders three synergistic effects via a full-pathway charge-dynamics regulation: (i) Ce-induced lattice distortion enhances ferroelectric polarization, reinforcing the polarization electric field for directional charge separation; (ii) band-edge reconstruction reduces both carrier effective masses and exciton binding energy, accelerating exciton dissociation and carrier transport; and (iii) the unpaired 4f1 electron of Ce3+ induces spin polarization, effectively lowering the spin-related kinetic barriers for H2O2 generation. Consequently, Ce-doped Bi3TiNbO9 delivers an H2O2 production rate of 1151.7 µmol g−1 h−1 in pure water, a 6.9-fold enhancement over pristine Bi3TiNbO9. Critically, applying a 300 mT external magnetic field further boosts the rate to 1831.2 µmol g−1 h−1, providing direct evidence for spin-polarization-controlled photocatalysis. H2O2 is selectively generated through synergistic 2e− oxygen reduction reaction (ORR) and water oxidation reaction (WOR) pathways, while the competing side reactions are effectively suppressed. This work demonstrates an integrated 4f-mediated charge–spin regulation strategy that couples charge separation with spin-dependent surface reaction kinetics for efficient H2O2 photosynthesis.
SN  - 2041-6520
SN  - 2041-6539
ER  -