Alkali metal modified carbon nitride enhance photocatalytic performance for highly selective oxidation of benzyl C(sp3)-H bonds

被引:18
|
作者
Qi, Qiqi [1 ]
Li, Yali [2 ]
Liu, Hao [1 ]
Li, Baoying [1 ]
Wang, Hong [1 ]
Lu, Yi [1 ]
Gao, Wei [1 ]
Tian, Yingjun [1 ]
Guo, Bingpeng [1 ]
Jia, Xiaofei [3 ]
Chen, Jianbin [1 ]
机构
[1] Qilu Univ Technol, Shandong Acad Sci, Sch Chem & Chem Engn, Shandong Prov Key Lab Mol Engn, Jinan 250353, Peoples R China
[2] Beijing Acad Sci & technol, Beijing Ctr Phys & Chem Anal, Inst Anal & testing, Beijing 100089, Peoples R China
[3] Qingdao Univ Sci & Technol, Coll Chem & Mol Engn, Key Lab Opt Elect Sensing & Analyt Chem Life Sci, MOE, Qingdao 266042, Peoples R China
基金
中国国家自然科学基金;
关键词
Photocatalysis; Alkali metal doping; Selective oxidation; Singlet oxygen; DOPED G-C3N4; HYDROGEN-PEROXIDE; OXYGEN; BENZALDEHYDE; ACTIVATION; NANOSHEETS; TOLUENE; SITES;
D O I
10.1016/j.apcatb.2022.121864
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
Photocatalytic selective oxidation of C(sp(3))-H bonds is an attractive strategy for synthesis of high value-added products due to the property of solar-driven and mild reaction conditions. However, improving photocatalytic activity and selectivity is still a grand challenge. Herein, we systematically compared the activity and selectivity for photocatalytic oxidation of 4-phenyltoluene by using the as-prepared photocatalysts. The results demonstrated that structure control and alkali metal modification could improve photocatalytic activity and selectivity by increasing the amount of singlet oxygen (1O2) molecules, which was proved by electron paramagnetic resonance (EPR) spectroscopy and phosphorescence (PH) spectroscopy. Moreover, no apparent decrease of conversion rate and selectivity during the 6 cycle runs indicated excellent stability of the prepared photo -catalysts. This work revealed a basic mechanism on the energy transfer process of excitons and developed a feasible strategy for the design of C3N4-based photocatalysts.
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页数:10
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