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<p>Achieving high specific surface area (HSSA) in graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) severely depolymerizes the molecular chain structure, resulting in sluggish carrier kinetic behaviors and thus moderated water purification performance in photocatalytic peroxymonosulfate (PMS) activation system. Herein, we report a versatile shear-repair strategy for fabricating ultrathin porous g-C<sub>3</sub>N<sub>4</sub> nanosheets with a thickness of 1.5 nm, HSSA (138.5 m<sup>2</sup> g<sup>−1</sup>), and highly polymerized molecular chains. This strategy accelerates exciton dissociation and charge carrier separation, with the exciton binding energy decreasing from 65.7 to 47.5 meV. Crucially, the electron-donating pollutant and electron-withdrawing PMS generate a microelectric field at the g-C<sub>3</sub>N<sub>4</sub> surface that activates PMS to generate <sup>1</sup>O<sub>2</sub> sustainably. Consequently, our catalyst exhibits an exceptional imidacloprid (IMD) removal performance with a rate constant of 0.405 min<sup>−1</sup> and remarkable PMS utilization efficiency (90% within 15 min). Moreover, under real conditions of sunlight irradiation, we observe an outstanding pollutants’ removal efficiency with a near-100% degradation rate over 20 days of continuous operation. Our work emphasizes the feasibility of synergistic molecular-level structural engineering for refining carrier kinetic behaviors in high-performance photocatalyst design.</p>

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Facilitating carrier kinetics in ultrathin porous carbon nitride through shear-repair strategy for peroxymonosulfate-assisted water purification

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月1日

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  • Hao Liu,
  • Bin Yang,
  • Guangfu Liao,
  • Baoyu Huang,
  • Jun Li,
  • Raul D. Rodriguez,
  • Xin Jia

摘要

Achieving high specific surface area (HSSA) in graphitic carbon nitride (g-C3N4) severely depolymerizes the molecular chain structure, resulting in sluggish carrier kinetic behaviors and thus moderated water purification performance in photocatalytic peroxymonosulfate (PMS) activation system. Herein, we report a versatile shear-repair strategy for fabricating ultrathin porous g-C3N4 nanosheets with a thickness of 1.5 nm, HSSA (138.5 m2 g−1), and highly polymerized molecular chains. This strategy accelerates exciton dissociation and charge carrier separation, with the exciton binding energy decreasing from 65.7 to 47.5 meV. Crucially, the electron-donating pollutant and electron-withdrawing PMS generate a microelectric field at the g-C3N4 surface that activates PMS to generate 1O2 sustainably. Consequently, our catalyst exhibits an exceptional imidacloprid (IMD) removal performance with a rate constant of 0.405 min−1 and remarkable PMS utilization efficiency (90% within 15 min). Moreover, under real conditions of sunlight irradiation, we observe an outstanding pollutants’ removal efficiency with a near-100% degradation rate over 20 days of continuous operation. Our work emphasizes the feasibility of synergistic molecular-level structural engineering for refining carrier kinetic behaviors in high-performance photocatalyst design.