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<p>Photocatalytic activation of molecular oxygen (O<sub>2</sub>) into reactive oxygen species (ROS) is pivotal for water purification, yet achieving selective ROS generation remains challenging. In this work, we successfully fabricated N-doped carbon-coated BiOCl (BNC) photocatalysts featuring abundant surface oxygen vacancies (OVs), a unique structure that synergistically enhances excitonic effects and promotes singlet oxygen (<sup>1</sup>O<sub>2</sub>) generation. The N-doped carbon layer synergistically with OVs boosts <sup>1</sup>O<sub>2</sub> generation by facilitating spin–orbit coupling, reducing the singlet–triplet energy gap by 36% to promote intersystem crossing, and enhancing O<sub>2</sub> chemisorption/activation by O–O bond lengthening to 1.52&#xa0;Å, resulting in a tenfold <sup>1</sup>O<sub>2</sub> yield increase over pristine BiOCl. Optimized BNC10 sample completely degraded ciprofloxacin in 60&#xa0;min under visible-light irradiation, with 6.9-fold higher rate constant, showed &gt; 87% removal in real waters. Toxicity assessments confirmed the low ecological risk of degradation intermediates, while mineralization experiments demonstrated 80% total organic carbon (TOC) removal. This work provides a novel strategy for excitonic regulation in 2D semiconductors, advancing the design of selective photocatalysts for sustainable environmental remediation.</p> Graphical Abstract <p>Boosted energy-transfer-mediated molecular oxygen activation by coating N-doped carbon layer endows BiOCl with high yield of <sup>1</sup>O<sub>2</sub> toward efficient degradation of various pollutants.</p> <p></p>

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Oxygen vacancies and N-doped carbon layer synergistically enhance singlet oxygen generation over BiOCl for efficient pollutant degradation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月23日

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  • Chenyu Zhang,
  • Zeyan Zhou,
  • Chenhong Wu,
  • Hao Zeng,
  • Qiongfang Wan,
  • Hui Li,
  • Hanbo Yu,
  • Haoliang Pang,
  • Jinhui Huang,
  • Xingzhong Yuan

摘要

Photocatalytic activation of molecular oxygen (O2) into reactive oxygen species (ROS) is pivotal for water purification, yet achieving selective ROS generation remains challenging. In this work, we successfully fabricated N-doped carbon-coated BiOCl (BNC) photocatalysts featuring abundant surface oxygen vacancies (OVs), a unique structure that synergistically enhances excitonic effects and promotes singlet oxygen (1O2) generation. The N-doped carbon layer synergistically with OVs boosts 1O2 generation by facilitating spin–orbit coupling, reducing the singlet–triplet energy gap by 36% to promote intersystem crossing, and enhancing O2 chemisorption/activation by O–O bond lengthening to 1.52 Å, resulting in a tenfold 1O2 yield increase over pristine BiOCl. Optimized BNC10 sample completely degraded ciprofloxacin in 60 min under visible-light irradiation, with 6.9-fold higher rate constant, showed > 87% removal in real waters. Toxicity assessments confirmed the low ecological risk of degradation intermediates, while mineralization experiments demonstrated 80% total organic carbon (TOC) removal. This work provides a novel strategy for excitonic regulation in 2D semiconductors, advancing the design of selective photocatalysts for sustainable environmental remediation.

Graphical Abstract

Boosted energy-transfer-mediated molecular oxygen activation by coating N-doped carbon layer endows BiOCl with high yield of 1O2 toward efficient degradation of various pollutants.