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<p>Photocatalytic lignin refinery into aromatic compounds represents a promising and sustainable strategy for the valorization of this biomass, although the low efficiency of photogenerated carrier separation may lead to poor bond cleavage activity, especially within the macromolecular natural lignin. Herein, we introduce a novel heterostructure photocatalyst by incorporating carbon-vacancy-rich graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) quantum dots (QDs) onto ZnIn<sub>2</sub>S<sub>4</sub> (ZIS) nanoflakes (ZIS@C<sub>3</sub>N<sub>4</sub> QDs). The carbon vacancies in g-C<sub>3</sub>N<sub>4</sub> QDs confer abundant electron-donating –NH<sub><i>x</i></sub> groups and unsaturated nitrogen sites, which synergistically enhance the separation of photogenerated electron-hole pairs within ZIS under an interfacial built-in electric field (IEF). Mechanism study reveals that the IEF, derived from Fermi energy level equilibration, is strengthened by the polarity of –NH<sub><i>x</i></sub> groups, thereby driving directional charge migration and enhancing the β–O–4 bond cleavage mediated by the generated hydrogen radicals <b>[H]</b>. Under the ZIS@C<sub>3</sub>N<sub>4</sub> QDs, photocatalytic cleavage of a typical lignin model compound achieves an impressive yield of acetophenone monomer for 77.76%, showcasing excellent catalytic performance. Furthermore, the as-designed photocatalyst effectively realizes the depolymerization of natural-like poplar lignin into corresponding ketones, producing a total of 19.52 wt% aromatic monomers. These results provide valuable guidance for the rational design of photocatalytic systems for converting renewable biomass feedstocks into high-value fine chemicals.</p>

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Enhanced interfacial electric field via carbon vacancy engineering in ZnIn2S4/g-C3N4 QDs heterostructure for efficient photocatalytic lignin refinery

  • 期刊论文

  • 发表日期：

    2026年3月19日

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  • Qingguo Zhou,
  • Jingxuan Zhang,
  • Ming Li,
  • Wenjing Bai,
  • Wenxiao Guo,
  • Ao Zhou,
  • Liyuan Gong,
  • Yongzhuang Liu,
  • Zupeng Chen,
  • Haipeng Yu,
  • Shuo Dou

摘要

Photocatalytic lignin refinery into aromatic compounds represents a promising and sustainable strategy for the valorization of this biomass, although the low efficiency of photogenerated carrier separation may lead to poor bond cleavage activity, especially within the macromolecular natural lignin. Herein, we introduce a novel heterostructure photocatalyst by incorporating carbon-vacancy-rich graphitic carbon nitride (g-C3N4) quantum dots (QDs) onto ZnIn2S4 (ZIS) nanoflakes (ZIS@C3N4 QDs). The carbon vacancies in g-C3N4 QDs confer abundant electron-donating –NHx groups and unsaturated nitrogen sites, which synergistically enhance the separation of photogenerated electron-hole pairs within ZIS under an interfacial built-in electric field (IEF). Mechanism study reveals that the IEF, derived from Fermi energy level equilibration, is strengthened by the polarity of –NHx groups, thereby driving directional charge migration and enhancing the β–O–4 bond cleavage mediated by the generated hydrogen radicals [H]. Under the ZIS@C3N4 QDs, photocatalytic cleavage of a typical lignin model compound achieves an impressive yield of acetophenone monomer for 77.76%, showcasing excellent catalytic performance. Furthermore, the as-designed photocatalyst effectively realizes the depolymerization of natural-like poplar lignin into corresponding ketones, producing a total of 19.52 wt% aromatic monomers. These results provide valuable guidance for the rational design of photocatalytic systems for converting renewable biomass feedstocks into high-value fine chemicals.