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Journal of Colloid and Interface Science

Journal of Colloid and Interface Science

IF: 9.4
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Dual-site and carbon-ring moiety modulation of polymeric carbon nitride for improved cooperative photocatalysis

Published:2 December 2024 DOI: 10.1016/j.jcis.2024.12.003 PMID: 39642557
Pengbo Li,?Yuanrong Zhang,?Haodi Liu,?Yanfen Fang,?Shuaitao Li,?Xun Hu,?Qifeng Chen

Abstract

The conjugated structure of graphitic polymeric carbon nitrides (GPCNs) has low efficiency in the photocatalytic hydrogen peroxide (H2O2) production, due to the electronic properties, band structure, and surface-active-sites. Herein, boron and carbon-ring modified GPCNs were synthesized with via a thermal condensation method, using melamine and phenylboronic acid as raw materials. The introduced boron atom, conjugated to the carbon atom in the heptazine moiety, and the adjacent nitrogen vacancy (VN) formed a dual-site, which not only modified the electronic properties but also promoted the adsorption and activation of molecular dioxygen; The carbon-ring introduced altered the band structure and electron distribution, which was proved by density functional theory (DFT) calculations. The co-modification promoted the conversion of dioxygen molecule to H2O2, coupled with oxidation of benzyl alcohol (BA) to benzaldehyde (BAD). The optimal activity was achieved over CN-B3 (1.87?mmol/(g·h)), which was about 4-fold higher than that of PCN (0.49?mmol/(g·h)). More interestingly, mechanism study revealed that the photocatalytic H2O2 generation was realized via a photon energy transfer route, that is, O2 molecule firstly was converted to a highly active singlet oxygen (1O2) intermediate, which was reduced by electrons to superoxide anions (O2-) and coupled with proton to form H2O2. This method provides a novel strategy to improve photocatalytic H2O2 and high value-added chemical production by regulating the microstructure and electronic structure of GPCNs through heteroatom and moiety co-modification.

Substances (8)

Materials
Procduct Name CAS Molecular Formula Supplier Price
Benzyl alcohol 100-51-6 C7H8O 1522 suppliers $5.00-$15264.00
Acetonitrile 75-05-8 C2H3N 1022 suppliers $61180.00
Melamine 108-78-1 C3H6N6 862 suppliers $5.00-$1593.90
Triethanolamine 102-71-6 C6H15NO3 857 suppliers $18.00-$4666.00
1,4-Benzoquinone 106-51-4 C6H4O2 555 suppliers $10.00-$7780.00
Furfuryl alcohol 98-00-0 C5H6O2 538 suppliers $25.65-$7920.65
potassium ferricyanide 13746-66-2 C6FeN6.3K 456 suppliers $10.00-$15160.00
Vanillyl alcohol 498-00-0 C8H10O3 386 suppliers $21.00-$4341.65

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