Journal
ACS APPLIED MATERIALS & INTERFACES
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c12038
Keywords
polymeric carbon nitride; fluorine/potassium modulation; layer configuration control; interlayer exciton dissociation; photosynthetic H2O2
Funding
- National Natural Science Foundation of China [21808089, 21806060]
- Natural Science Foundation of Jiangsu Province [BK20211322]
- China Postdoctoral Science Foundation [2021M691331, 2019M661750]
- Postdoctoral Fund of Jiangsu Province [2021K371C]
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In this study, a layered heterojunction of polymeric carbon nitride (PCN) with heptazine/triazine and fluorine/potassium (F/K) dual sites (FKHTCN) was constructed to enhance the photocatalytic production of hydrogen peroxide (H2O2). The introduction of F/K not only improved the charge separation efficiency but also optimized the adsorption of oxygen molecules and intermediate *OOH during H2O2 production. The FKHTCN exhibited a significantly higher H2O2 production rate (15 times higher than PCN) and showed potential for practical applications in environmental remediation.
Photocatalytic hydrogen peroxide (H2O2) production will become a burgeoning strategy for solar energy utilization by selective oxygen reduction reaction (ORR). Polymeric carbon nitride (PCN) shows relatively high two-electron ORR selectivity for H2O2 production but still limited low H2O2 production efficiency due to slow exciton dissociation. Herein, we constructed a heptazine/triazine layer stacked carbon nitride heterojunction with fluorine/potassium (F/K) dual sites (FKHTCN). The introduction of F/K not only can regulate layer components to enhance the charge separation efficiency but, more importantly, also optimize the adsorption of surface oxygen molecules and intermediate *OOH during H2O2 production. Consequently, FKHTCN efficiently improves the photocatalytic H2O2 production rate up to 3380.9 mu mol h(-1) g(-1), nearly 15 times higher than that of traditional PCN. Moreover, a production-utilization cascade system was designed to explore their practical application in environmental remediation. This work lays out the importance of engineering a layer-stacked configuration and active sites for enhancing photocatalysis.
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