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<p>Photo-assisted lithium–sulfur batteries (PALSBs) offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs. However, designing an efficient photoelectrode for practical implementation remains a significant challenge. Herein, we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs. Specifically, polypyrrole (PPy) is in situ vapor-phase polymerized on the surface of N-doped TiO<sub>2</sub> nanorods supported on carbon cloth (N-TiO<sub>2</sub>/CC), thereby forming a well-defined p–n heterojunction. This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field. Thus, the PPy@N-TiO<sub>2</sub>/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur, enabling ultrafast sulfur redox dynamics, as convincingly validated by both theoretical simulations and experimental results. Consequently, the PPy@N-TiO<sub>2</sub>/CC PALSB achieves a high discharge capacity of 1653&#xa0;mAh&#xa0;g<sup>−1</sup>, reaching 98.7% of the theoretical value. Furthermore, 5&#xa0;h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333&#xa0;mAh&#xa0;g<sup>−1</sup>, achieving dual-mode energy harvesting capabilities. This work successfully integrates solar energy conversion and storage within a rechargeable battery system, providing a promising strategy for sustainable energy storage technologies.</p>

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Ultrafast Sulfur Redox Dynamics Enabled by a PPy@N-TiO2 Z-Scheme Heterojunction Photoelectrode for Photo-Assisted Lithium–Sulfur Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月1日

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  • Fei Zhao,
  • Yibo He,
  • Xuhong Li,
  • Ke Yang,
  • Shuo Chen,
  • Yuanzhi Jiang,
  • Xue-Sen Wang,
  • Chunyuan Song,
  • Xuqing Liu

摘要

Photo-assisted lithium–sulfur batteries (PALSBs) offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs. However, designing an efficient photoelectrode for practical implementation remains a significant challenge. Herein, we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs. Specifically, polypyrrole (PPy) is in situ vapor-phase polymerized on the surface of N-doped TiO2 nanorods supported on carbon cloth (N-TiO2/CC), thereby forming a well-defined p–n heterojunction. This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field. Thus, the PPy@N-TiO2/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur, enabling ultrafast sulfur redox dynamics, as convincingly validated by both theoretical simulations and experimental results. Consequently, the PPy@N-TiO2/CC PALSB achieves a high discharge capacity of 1653 mAh g−1, reaching 98.7% of the theoretical value. Furthermore, 5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g−1, achieving dual-mode energy harvesting capabilities. This work successfully integrates solar energy conversion and storage within a rechargeable battery system, providing a promising strategy for sustainable energy storage technologies.