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<p>Conventional syntheses of tocopheryl acetate rely on strong Brønsted/Lewis acids and energy-intensive conditions. Here we report a visible-light photocatalytic route using graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) engineered by precursor control, P/S co-doping, metal loading (Cu, V, Zn, Ni), and nanosheet formation. Structural characterization by SEM and TEM revealed that P/S co-doping and exfoliation produced highly corrugated nanosheets with increased porosity, abundant edge sites, and reduced interlayer stacking. XRD analysis confirmed the preservation of the g-C<sub>3</sub>N<sub>4</sub> framework with slight distortion upon doping, while HRTEM showed lattice disorder and defect formation that are beneficial for charge trapping and transfer. In ethanol/H<sub>2</sub>O<sub>2</sub> under a 40&#xa0;W lamp, P/S@g-C<sub>3</sub>N<sub>4</sub> affords a 76.26% yield with 99.80% selectivity; no formation occurs in the dark. Screening identifies 5&#xa0;mg mL<sup>−1</sup> substrate, 4&#xa0;mg catalyst, and 45&#xa0;°C as optimal, while yields decline above 55&#xa0;°C. The catalyst is reusable for 20 cycles with slight loss from handling. DRS results showed that the absorption capacity of P/S@g-C<sub>3</sub>N<sub>4</sub> to visible light was significantly higher than that of g-C<sub>3</sub>N<sub>4</sub>. And compared with g-C<sub>3</sub>N<sub>4</sub>, the E<sub>g</sub> value of P/S@g-C<sub>3</sub>N<sub>4</sub> is significantly narrowed form 2.71&#xa0;eV to 2.42&#xa0;eV. Mechanistic analysis indicates P/S sites and heterointerfaces enhance H<sub>2</sub>O<sub>2</sub> activation, oxidize ethanol to acetaldehyde, and channel coupling with a phenoxyl intermediate from tocopherol. This acid-free strategy offers a scalable route to tocopheryl acetate.</p>

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Highly Selective Visible-Light Photocatalytic Synthesis of Tocopheryl Acetate Over Heterostructured g-C3N4

  • 期刊论文

  • 发表日期：

    2026年6月25日

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  • Yulin Shan,
  • Junjie Li,
  • Chao Li,
  • Zixuan Bai,
  • Binglin Li,
  • Ziwei Liu

摘要

Conventional syntheses of tocopheryl acetate rely on strong Brønsted/Lewis acids and energy-intensive conditions. Here we report a visible-light photocatalytic route using graphitic carbon nitride (g-C3N4) engineered by precursor control, P/S co-doping, metal loading (Cu, V, Zn, Ni), and nanosheet formation. Structural characterization by SEM and TEM revealed that P/S co-doping and exfoliation produced highly corrugated nanosheets with increased porosity, abundant edge sites, and reduced interlayer stacking. XRD analysis confirmed the preservation of the g-C3N4 framework with slight distortion upon doping, while HRTEM showed lattice disorder and defect formation that are beneficial for charge trapping and transfer. In ethanol/H2O2 under a 40 W lamp, P/S@g-C3N4 affords a 76.26% yield with 99.80% selectivity; no formation occurs in the dark. Screening identifies 5 mg mL−1 substrate, 4 mg catalyst, and 45 °C as optimal, while yields decline above 55 °C. The catalyst is reusable for 20 cycles with slight loss from handling. DRS results showed that the absorption capacity of P/S@g-C3N4 to visible light was significantly higher than that of g-C3N4. And compared with g-C3N4, the Eg value of P/S@g-C3N4 is significantly narrowed form 2.71 eV to 2.42 eV. Mechanistic analysis indicates P/S sites and heterointerfaces enhance H2O2 activation, oxidize ethanol to acetaldehyde, and channel coupling with a phenoxyl intermediate from tocopherol. This acid-free strategy offers a scalable route to tocopheryl acetate.