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Molecular engineering of g-C3N4 with spatial charge separation for enhancing photocatalytic performances
Materials Chemistry Frontiers ( IF 7 ) Pub Date : 2022-06-10 , DOI: 10.1039/d2qm00184e
Mingrui Guo 1 , Meng Chen 1 , Jixiang Xu 1 , Jing Wang 1 , Lei Wang 1
Affiliation  

The intramolecular doping of donor units or acceptor units in carbon nitride (g-C3N4, CN) is regarded as an effective method for regulating electron structure and enhancing the catalytic activity of CN. Herein, benzene rings and eosin Y (EY) co-grafted CN with carbon vacancies (EY-PhCN) was prepared by calcining a supermolecular precursor consisting of melamine, cyanuric acid, and benzonquanmine followed by covalently hooking the EY. Theoretical and experimental results demonstrated the directional electron transfer, spatially isolated electron–hole pairs and increased light response in the resulting ultrathin holey EY-PhCN. An optimal H2 production rate of 4.44 mmol g−1 h−1 was obtained over the 1%Pt-loaded EY-PhCN catalyst. The corresponding apparent quantum yield was 27.38% at 420 nm. Moreover, the EY-PhCN exhibited high CO2 reduction rate with H2O. The yields of CO and CH4 were 61.91 and 13.75 μmol g−1, respectively within 5 h light irradiation, higher than that of CN (CO: 24.60 μmol g−1, CH4: 8.51 μmol g−1). The work may give new insight into associating carbon vacancies and edge decoration on CN to achieve remarkably enhanced photocatalytic activity.

中文翻译:

g-C3N4的分子工程与空间电荷分离以提高光催化性能

在氮化碳(gC 3 N 4 , CN)中分子内掺杂施主单元或受主单元被认为是调节电子结构和提高CN催化活性的有效方法。在此,通过煅烧由三聚氰胺、氰尿酸和苯全胺组成的超分子前体,然后共价连接 EY,制备了苯环和伊红 Y (EY) 共接枝 CN 与碳空位 (EY-PhCN)。理论和实验结果证明了定向电子转移、空间隔离的电子-空穴对和在所得超薄孔 EY-PhCN 中增加的光响应。4.44 mmol g -1 h -1的最佳H 2产率在负载 1% Pt 的 EY-PhCN 催化剂上获得。在 420 nm 处相应的表观量子产率为 27.38%。此外,EY-PhCN在H 2 O的作用下表现出较高的CO 2还原率。在光照5小时内,CO和CH 4的产率分别为61.91和13.75 μmol g -1,高于CN(CO:24.60 μmol)。 g -1,CH 4:8.51 μmol g -1 )。这项工作可能会为将碳空位与 CN 上的边缘装饰相关联以实现显着增强的光催化活性提供新的见解。
更新日期:2022-06-15
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