Tailoring Phenol Photomineralization Pathway Over Polymeric Carbon Nitride With Cyano Group Multifunctional Active Sites

APPLIED CATALYSIS B-ENVIRONMENTAL(2021)

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摘要
The electronic and interfacial properties of catalysts play vital roles in tailoring catalytic performance. Here, we report that the modification of polymeric carbon nitride (PCN) with cyano group (-CN) can achieve excellent catalytic performance in mineralization of phenol. The -CN site not only enhances the adsorption and activation of molecular O-2 for efficient H2O2 production, but also improves the absorption capability of PCN for phenol in aqueous solution by tuning surface charge states. Subsequently, the surficial adsorbed phenol acts as holes scavenger which promotes the separation efficiency of photogenerated carriers in PCN and in turn facilitates the in-situ decomposition of H2O2 to (OH)-O-center dot. This reduces the uncontrollable decomposition of H2O2 to (OH)-O-center dot and inhibits the polymerization of phenolic compounds. The active sites of catalyst, O-2 transformation state and pathway on the catalyst surface as well as the firstly attacked sites of phenol are confirmed respectively by in-situ DRIFT spectra, scavengers and Bader charge analysis.
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关键词
Cyano group, Polymeric carbon nitride, Tailoring photocatalytic H2O2 formation, Inhibiting phenol polymerization, Reactive oxygen species
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