<p>Molecular design of novel precursors represents a strategic approach to mitigating severe charge recombination in g-C<sub>3</sub>N<sub>4</sub>. Distinct from conventional high-temperature thermal polymerization, this work develops novel precursors through low-temperature hydrothermal assembly of melamine-cyanuric acid supramolecule with hexamethylenetetramine doping. After the calcination of modified precursors, the obtained g-C<sub>3</sub>N<sub>4</sub> has a porous structure and an ultra-high specific surface area. Advanced characterizations confirm the reduced layer stacking, the disrupted <i>π-π</i> conjugated structure, and critically, the accelerated charge transport efficiency. Remarkably, the modified g-C<sub>3</sub>N<sub>4</sub> achieves a 22 times enhancement in visible-light-driven hydrogen evolution (<i>λ</i>&gt;400 nm) compared to pristine g-C<sub>3</sub>N<sub>4</sub>, which is among the highest improvements reported for supramolecular modified g-C<sub>3</sub>N<sub>4</sub> systems. This molecular engineering strategy for precursors establishes a new approach to designing high-performance photocatalysts.</p>

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Molecular-doped Precursor Derived Porous g-C3N4 for Photocatalytic H2 Production

  • Binjiang Zhai,
  • Yuzhou Jiang,
  • Shichao Zong,
  • Mingzhi Wang,
  • Zixin Wang,
  • Hui Jin,
  • Yanbing Liu,
  • Xing Kang,
  • Jinwen Shi

摘要

Molecular design of novel precursors represents a strategic approach to mitigating severe charge recombination in g-C3N4. Distinct from conventional high-temperature thermal polymerization, this work develops novel precursors through low-temperature hydrothermal assembly of melamine-cyanuric acid supramolecule with hexamethylenetetramine doping. After the calcination of modified precursors, the obtained g-C3N4 has a porous structure and an ultra-high specific surface area. Advanced characterizations confirm the reduced layer stacking, the disrupted π-π conjugated structure, and critically, the accelerated charge transport efficiency. Remarkably, the modified g-C3N4 achieves a 22 times enhancement in visible-light-driven hydrogen evolution (λ>400 nm) compared to pristine g-C3N4, which is among the highest improvements reported for supramolecular modified g-C3N4 systems. This molecular engineering strategy for precursors establishes a new approach to designing high-performance photocatalysts.