To promote charge transfer and separation for efficient photocatalysis,a direct Z-scheme heterostructure was constructed by coupling polymeric carbon nitride(PCN) and WO_(3).Interestingly,the obtained PCN/WO_(3)Z-sche...To promote charge transfer and separation for efficient photocatalysis,a direct Z-scheme heterostructure was constructed by coupling polymeric carbon nitride(PCN) and WO_(3).Interestingly,the obtained PCN/WO_(3)Z-scheme heterostructure could photocataly tic ally produce hydrogen and value-added chemicals(e.g.,formate and acetate) by reforming of plastic polylactic acid(PLA) in alkaline aqueous condition.By optimizing WO_(3) contents and reaction conditions,the obtained PCN/WO_(3)heterostructure exhibits much increased photocatalytic activity for PLA photoreforming under visible light,with hydrogen evolution rate reaching 402.90 μmol·g~(-1)·h~(-1),which is 3.5 times that of PCN.It is revealed that the Z-scheme charge transfer between PCN and WO_(3) mainly contributes to the promoted charge separation and thus the improved photocatalytic activity.Moreover,with h+and·OH experimentally evidenced as the predominant active species,a possible reaction pathway for the reforming of PLA into value-added chemicals(e.g.,formate and acetate)over PCN/WO_(3) Z-scheme heterostructure is cleared by monitoring the reaction intermediates and radicals.This work paves a carbon neutrality and scalable route toward the synergistical production of hydrogen and value-added chemicals by utilizing and recycling plastic waste.展开更多
基金financially supported by the National Natural Science Foundation of China (No.52225606)。
文摘To promote charge transfer and separation for efficient photocatalysis,a direct Z-scheme heterostructure was constructed by coupling polymeric carbon nitride(PCN) and WO_(3).Interestingly,the obtained PCN/WO_(3)Z-scheme heterostructure could photocataly tic ally produce hydrogen and value-added chemicals(e.g.,formate and acetate) by reforming of plastic polylactic acid(PLA) in alkaline aqueous condition.By optimizing WO_(3) contents and reaction conditions,the obtained PCN/WO_(3)heterostructure exhibits much increased photocatalytic activity for PLA photoreforming under visible light,with hydrogen evolution rate reaching 402.90 μmol·g~(-1)·h~(-1),which is 3.5 times that of PCN.It is revealed that the Z-scheme charge transfer between PCN and WO_(3) mainly contributes to the promoted charge separation and thus the improved photocatalytic activity.Moreover,with h+and·OH experimentally evidenced as the predominant active species,a possible reaction pathway for the reforming of PLA into value-added chemicals(e.g.,formate and acetate)over PCN/WO_(3) Z-scheme heterostructure is cleared by monitoring the reaction intermediates and radicals.This work paves a carbon neutrality and scalable route toward the synergistical production of hydrogen and value-added chemicals by utilizing and recycling plastic waste.
