Nitrogen vacancy engineered graphitic C3N4-based polymers for photocatalytic oxidation of aromatic alcohols to aldehydes

被引:308
作者
Ding, Jing [1 ]
Xu, Wei [1 ]
Wan, Hui [1 ]
Yuan, Dashui [1 ]
Chen, Chong [1 ]
Wang, Lei [1 ]
Guan, Guofeng [1 ]
Dai, Wei-Lin [2 ,3 ]
机构
[1] Nanjing Tech Univ, Jiangsu Natl Synerget Innovat Ctr Adv Mat, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China
[2] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
[3] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China
基金
中国国家自然科学基金;
关键词
Graphitic carbon nitride; Nitrogen vacancy; Photocatalysis; Aromatic alcohols; Organic dyes; CARBON NITRIDE NANOSHEETS; VISIBLE-LIGHT; BENZYL ALCOHOL; PHOTOREDOX CATALYSIS; SELECTIVE OXIDATION; AEROBIC OXIDATION; TIO2; NANOSHEETS; WO3; NANORODS; METAL-FREE; G-C3N4;
D O I
10.1016/j.apcatb.2017.09.048
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Vacancy defect in the semiconductors plays an important role in the improvement of the electronic structure and the increase of specific reaction sites for reactant molecules, and consequently enhancing the photocatalytic activity of semiconductor photocatalysts. Through high -temperature thermal condensation of a nitric acid pretreated melamine precursor, nitrogen vacancies were successfully introduced in the framework of g-C3N4. The nitrogen vacancies located at the uncondensed terminal Mix lattice sites were conducive to the enhancement of optical absorption, the improvement of the separation efficiency of the photogenerated charge carrier and the increase of surface area, which was beneficial to the photocatalytic oxidation process. More significantly, the novel CNNA(X) were used as efficient photocatalysts in the green process of aromatic aldehydes from the photocatalytic selective oxidation of aromatic alcohols and the photocatalytic degradation of organic pollutants. CNNA(X) samples exhibited enhanced photocatalytic activity and excellent recyclability and stability. The 68.3% benzyl alcohol conversion and almost 100% selectivity was observed for the CNNA (0.9) photocatalyst, higher than that of pure g-C3N4. Meanwhile, CNNA (0.9) showed superior photocatalytic degradation performance of organic dyes (RhB and MO). Furthermore, the underlying photocatalytic oxidation mechanism was proposed by the controlled experiments using radical scavengers.
引用
收藏
页码:626 / 634
页数:9
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