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Modulation of Lewis acidic-basic sites for efficient photocatalytic H2O2 production over potassium intercalated tri-s-triazine materials
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-06-09 , DOI: 10.1016/j.apcatb.2020.119225
Jingzhen Zhang , Chunyang Yu , Junyu Lang , Yongfeng Zhou , Baoxue Zhou , Yun Hang Hu , Mingce Long

Photocatalytic H2O2 production (PHOP) on graphitic carbon nitride (GCN) at neutral pHs is limited by the sluggish oxidation of sacrificial alcohols and insufficient protons. In our work, the PHOP over a series of K intercalated triazine (KTCN) or tri-s-triazine units (KTTCN) reached 11–32 folds of GCN in the presence of only 0.5 vol% isopropanol, and a positive correlation between the H2O2 production and the K contents was found. The critical role of K was revealed as that K intercalation creates Lewis acidic sites for isopropanol adsorption and strengthens Lewis basic sites for hydrogen abstraction and proton release. The improved alcohol oxidation and enhanced O2 chemisorption synergistically result in dramatically accelerated PHOP over KTTCN. The findings provide the understanding of the preliminary active site dependent PHOP mechanism and bring insights for design of carbon nitride polymers with desirable photocatalytic performance.



中文翻译:

路易斯酸碱性位点的调制,可在钾插层的三-s-三嗪材料上有效地光催化生产H 2 O 2

牺牲性醇的缓慢氧化和质子不足限制了石墨碳氮化物(GCN)在中性pH值下光催化H 2 O 2的产生(PHOP)。在我们的工作中,在仅存在0.5%体积%异丙醇的情况下,一系列K插层三嗪(KTCN)或三-s-三嗪单元(KTTCN)的PHOP达到GCN的11–32倍,并且H与H之间呈正相关产生2 O 2,发现钾含量。揭示了K的关键作用,因为K的插入为异丙醇吸附创造了Lewis酸性位点,并增强了Lewis碱性位点的氢提取和质子释放。改善的醇氧化和增强的O 2化学吸附协同作用导致PHOP大大超过KTTCN。这些发现提供了对初步的依赖于活性位点的PHOP机制的理解,并为具有所需光催化性能的氮化碳聚合物的设计提供了见识。

更新日期:2020-06-09
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