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<p>The production of ultra-low sulfur clean fuels holds global significance for improving energy efficiency and reducing environmental pollution. Photocatalytic aerobic oxidative desulfurization (PODS) offers an attractive approach to efficiently remove refractory heterocyclic aromatic sulfur compounds under mild conditions. However, the sluggish charge dynamics, insufficient molecule activation, and slow mass transfer within photocatalysts restrict the overall desulfurization efficiency, hindering the widespread application of this technology. Herein, we developed a defective g-C<sub>3</sub>N<sub>4</sub> (M<sub>1</sub>U<sub>3</sub>CN) photocatalyst with bridged N<sub>3C</sub> vacancies and hierarchical porous structures to address these limitations. This catalyst not only demonstrates outstanding dibenzothiophene (DBT) removal efficiency of 99.6% for model oil with high conversion and selectivity but also achieves complete sulfur removal from gasoline as well as 96.7% sulfur removal for distilled diesel at room temperature, successfully achieving ultradeep aerobic oxidative desulfurization. The introduction of rich N<sub>3C</sub> vacancies and abundant micro-meso-macroporous distribution in M<sub>1</sub>U<sub>3</sub>CN enhances kinetic efficiencies by promoting charge carrier separation, mass transfer, and molecular activation simultaneously; resulting in exceptional PODS performance. This work provides a collaborative strategy to overcome kinetic challenges in aerobic oxidative desulfurization <i>via</i> defect and structural engineering of the catalyst.</p>

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Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization

  • 期刊论文

  • 发表日期：

    2025年1月2日

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  • Yina Nie,
  • Weijie Yang,
  • Xin Wang,
  • Xiang Li,
  • Lele Wei,
  • Xiaolin Bai,
  • Lin Liu,
  • Feng Fu,
  • Jun Wan

摘要

The production of ultra-low sulfur clean fuels holds global significance for improving energy efficiency and reducing environmental pollution. Photocatalytic aerobic oxidative desulfurization (PODS) offers an attractive approach to efficiently remove refractory heterocyclic aromatic sulfur compounds under mild conditions. However, the sluggish charge dynamics, insufficient molecule activation, and slow mass transfer within photocatalysts restrict the overall desulfurization efficiency, hindering the widespread application of this technology. Herein, we developed a defective g-C3N4 (M1U3CN) photocatalyst with bridged N3C vacancies and hierarchical porous structures to address these limitations. This catalyst not only demonstrates outstanding dibenzothiophene (DBT) removal efficiency of 99.6% for model oil with high conversion and selectivity but also achieves complete sulfur removal from gasoline as well as 96.7% sulfur removal for distilled diesel at room temperature, successfully achieving ultradeep aerobic oxidative desulfurization. The introduction of rich N3C vacancies and abundant micro-meso-macroporous distribution in M1U3CN enhances kinetic efficiencies by promoting charge carrier separation, mass transfer, and molecular activation simultaneously; resulting in exceptional PODS performance. This work provides a collaborative strategy to overcome kinetic challenges in aerobic oxidative desulfurization via defect and structural engineering of the catalyst.