Artigo Revisado por pares

Dual P-doped-site modified porous g-C3N4 achieves high dissociation and mobility efficiency for photocatalytic H2O2 production

2023; Elsevier BV; Volume: 461; Linguagem: Inglês

10.1016/j.cej.2023.142140

ISSN

1873-3212

Autores

Guiyang Yu, Ke Gong, Chuanwang Xing, Lan Hu, Haibin Huang, Lejie Gao, Debao Wang, Xiyou Li,

Tópico(s)

Covalent Organic Framework Applications

Resumo

Organic semiconductor under photoexcitation could generate abundant strong-binding Frenkel excitons and inevitably suffer from low dissociation efficiency (<1%) and poor mobility ability, which severely suppresses the efficient utilization of photogenerated charges and corresponding activity. Herein, a dual P-doping strategy is proposed in bay and corner sites implanted polymeric carbon nitride (PCN-D) for visible-driven H2O2 production. The dual P doping breaks localized electron state around original symmetric heptazine units and weakens the binding energy between electrons and holes, increasing dissociation efficiency to reach 11.9% with 20-fold improvement. In addition, the conductivity ability of PCN-D, including formed carrier charge concentration and mobility, achieves 13-fold and 7-fold improvement, which facilitates the charge transfer and separation. The proposed dual doped-P-site strategy, with the blessing of porous structure, provides plentiful active center for effective adsorption and activation of O2 molecule, further accelerating reaction progress and achieving six-times increase of photocatalytic H2O2 production rate. This work provides in-depth insight into the importance of dual P-doping to optimize kinetic behavior of photogenerated charges and opens an avenue to the multiscale doping-modulation of semiconductor with high efficiency solar energy conversion.

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