<p>Layered polymer suffers from a transfer barrier of photogenerated carriers resulting from the lack of interlamellar connection channels and intralayer disorder. Herein, a layer-stacked crystalline carbon nitride nanorod resembling an accordion (A-CNR) grafted abundant interlamellar oxygen-containing groups is ingeniously designed to break through the transfer barrier between layers without inserting any extra impurities. Density functional theory reveals that electrons are enriched near the oxygen-containing groups, promoting the extension and coupling of interlayer electron clouds. This reduces the interlamellar electrostatic potential barrier from 5.38 to 2.74 eV. Remarkably, the groups not only establish interlayer bridges but also guide carriers to the bridge entrance, further enhancing interlayer carrier transfer. Additionally, the intralayer carrier separation and transfer are also improved, profiting from the asymmetrical charge distribution and high crystallinity. A-CNR exhibits impressive photoelectric properties and photocatalytic water disinfection capability. Within 18 min irradiation, over 10<sup>6</sup> colony-forming units (CFU)/mL of bacteria are completely inactivated. Moreover, A-CNR can be dispersed in water over a long period benefiting from the introduced oxygen-containing groups, making it suitable for photocatalysis in the aqueous phase. The work provides a feasible and effective strategy to overcome the inherent barrier of layered polymeric photocatalysts.</p>

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Enhancing the interlamellar carrier transfer via oxygen-containing groups in layer-stacked carbon nitride nanorod for superior photocatalytic disinfection

  • Fengming Hou,
  • Wei Wei,
  • Ruirui Hou,
  • Rujing Shen,
  • Xianghong Niu,
  • Zhipeng Guo,
  • Yihang Li,
  • Xiuyun Zhang,
  • Ang Wei

摘要

Layered polymer suffers from a transfer barrier of photogenerated carriers resulting from the lack of interlamellar connection channels and intralayer disorder. Herein, a layer-stacked crystalline carbon nitride nanorod resembling an accordion (A-CNR) grafted abundant interlamellar oxygen-containing groups is ingeniously designed to break through the transfer barrier between layers without inserting any extra impurities. Density functional theory reveals that electrons are enriched near the oxygen-containing groups, promoting the extension and coupling of interlayer electron clouds. This reduces the interlamellar electrostatic potential barrier from 5.38 to 2.74 eV. Remarkably, the groups not only establish interlayer bridges but also guide carriers to the bridge entrance, further enhancing interlayer carrier transfer. Additionally, the intralayer carrier separation and transfer are also improved, profiting from the asymmetrical charge distribution and high crystallinity. A-CNR exhibits impressive photoelectric properties and photocatalytic water disinfection capability. Within 18 min irradiation, over 106 colony-forming units (CFU)/mL of bacteria are completely inactivated. Moreover, A-CNR can be dispersed in water over a long period benefiting from the introduced oxygen-containing groups, making it suitable for photocatalysis in the aqueous phase. The work provides a feasible and effective strategy to overcome the inherent barrier of layered polymeric photocatalysts.