<p>Low surface photogenerated charge concentration is a critical limitation hindering conventional graphitic carbon nitride (CN) from efficiently reducing CO<sub>2</sub> to high-value products. In this work, a pollution-free oxygen oxidation strategy was devised to enhance the surface charge enrichment sites of CN. This approach led to the successful fabrication of a tubular CN photocatalyst functionalized with oxygen-containing groups (C–O–C and C–OH), named O-TCN. The introduction of oxygen functional groups not only effectively widen the light absorption range and narrowed the bandgap but also optimized the surface electronic structure, realizing substantial photogenerated charge accumulation on the O-TCN surface. Photocatalytic performance evaluations revealed that O-TCN achieved exceptional catalytic activity and selectivity in CO<sub>2</sub> reduction, stably converting CO<sub>2</sub> to CO. The average CO yield of O-TCN reaches 49.8 µmol g<sup>−1</sup> h<sup>−1</sup>, representing enhancements of 5.5-fold and 7.7-fold compared to TCN and the classical bulk CN, respectively. This work highlights the potential of surface oxygen functionalization as a powerful strategy to boost the photocatalytic activity of CN-based materials, offering new insights for advancing sustainable energy conversion technologies.</p>

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Boosting photogenerated charge accumulation of oxidated carbon nitride nanotubes for efficient CO2 photoreduction

  • Weidong Hou,
  • Yuexia Li,
  • Kang Wang,
  • Huazhang Guo,
  • Baohua Zhang,
  • Liang Wang

摘要

Low surface photogenerated charge concentration is a critical limitation hindering conventional graphitic carbon nitride (CN) from efficiently reducing CO2 to high-value products. In this work, a pollution-free oxygen oxidation strategy was devised to enhance the surface charge enrichment sites of CN. This approach led to the successful fabrication of a tubular CN photocatalyst functionalized with oxygen-containing groups (C–O–C and C–OH), named O-TCN. The introduction of oxygen functional groups not only effectively widen the light absorption range and narrowed the bandgap but also optimized the surface electronic structure, realizing substantial photogenerated charge accumulation on the O-TCN surface. Photocatalytic performance evaluations revealed that O-TCN achieved exceptional catalytic activity and selectivity in CO2 reduction, stably converting CO2 to CO. The average CO yield of O-TCN reaches 49.8 µmol g−1 h−1, representing enhancements of 5.5-fold and 7.7-fold compared to TCN and the classical bulk CN, respectively. This work highlights the potential of surface oxygen functionalization as a powerful strategy to boost the photocatalytic activity of CN-based materials, offering new insights for advancing sustainable energy conversion technologies.