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Li, Mengqiao; Zheng, Qinmin; Durkin, David P.; Chen, Hanning; Shuai, Danmeng
Journal of hazardous materials, 08/2022, Volume: 436, Issue: CJournal Article
Solar-driven photocatalytic generation of H2O2 over metal-free catalysts is a sustainable approach for value-added chemical production. Here, we synthesized chlorine-doped graphitic carbon nitride (Cl-doped g-C3N4) through a solvothermal method to effectively produce H2O2 with a rate of 1.19 ± 0.06 µM min−1 under visible light irradiation, which was improved by 104 times compared to pristine g-C3N4. Continuous net production of H2O2 was realized at a rate of 2.78 ± 0.10 µM min−1 up to 54 h with isopropanol as the hole scavenger, whereas H2O2 production was only sustained for ~ 6 h without scavengers. Both molecular simulations and advanced spectroscopic characterizations elucidated that the Cl dopant increased the charge transfer rate, decreased the bandgap, and reduced the activation energy of the rate-limiting step of O2 reduction, all of which favored H2O2 production. This work implemented a novel metal-free photocatalyst for sustainable H2O2 production and elucidated the mechanism for promoting H2O2 production that can guide future photoreactive nanomaterial design. Display omitted •Cl-doped g-C3N4 was synthesized via a solvothermal method.•Cl dopant decreased the g-C3N4 bandgap and promoted charge transfer.•Cl dopant lowered the activation energy of the rate-determining step in H2O2 formation.•In the presence of isopropanol H2O2 was continuously produced on Cl-doped g-C3N4.
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