光催化
材料科学
兴奋剂
选择性
石墨氮化碳
催化作用
电子
合理设计
纳米技术
光化学
双重角色
光电子学
化学工程
组合化学
有机化学
化学
物理
工程类
量子力学
作者
Gang Wang,Rong Huang,Jiangwei Zhang,Junjie Mao,Dingsheng Wang,Yadong Li
标识
DOI:10.1002/adma.202105904
摘要
The separation efficiency of photo-generated carriers is still a great challenge that restricts the practical application of photocatalytic technology. The design of spatial separation path for photo-generated carriers at atomic level provides an innovative approach to address this challenge. Herein, a facile dual atomic sites strategy, consisting of Cu-N4 and C-S-C active moieties decorated on polymeric carbon nitride (Cu SAs/p-CNS) is reported to simultaneously achieve the highly efficient separation of photo-generated electrons and holes for boosting photocatalytic performance. As a proof of concept, the Cu SAs/p-CNS is successfully applied to the photo-oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF), which exhibits 77.1% HMF conversion and 85.6% DFF selectivity under visible light irradiation. The activity is considerably higher than that of bulk p-CN, S doped p-CN, and p-CN supported Cu single atom catalysts. Theoretical calculations and experimental results suggest that, during photocatalytic reaction, the isolated Cu-N4 sites directly capture photo-generated electrons, while the surrounding S atoms bear photo-generated holes, which synergistically facilitates the separation of photo-generated carriers and thus results in enhanced photocatalytic activity. This study provides a new perspective for the rational design of high performance photocatalysts at atomic level.
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