Citation: Yang Fan, Chu Xiaoyu, Sun Jianhui, Zhang Yuhang, Li Zhijun, Liu Haiyue, Bai Linlu, Qu Yang, Jing Liqiang. Efficient singlet oxygen generation by excitonic energy transfer on ultrathin g-C₃N₄ for selective photocatalytic oxidation of methyl-phenyl-sulfide with O₂[J]. Chinese Chemical Letters, ;2020, 31(10): 2784-2788. doi: 10.1016/j.cclet.2020.07.033 shu

Efficient singlet oxygen generation by excitonic energy transfer on ultrathin g-C₃N₄ for selective photocatalytic oxidation of methyl-phenyl-sulfide with O₂

Yang Fan ^a ,
Chu Xiaoyu ^a,b ,
Sun Jianhui ^a,*, ,
Zhang Yuhang ^a ,
Li Zhijun ^a ,
Liu Haiyue ^a ,
Bai Linlu ^a,b ,
Qu Yang ^a,*, ,
Jing Liqiang ^a,*,

a.
Department Key Laboratory of Functional Inorganic Materials Chemistry (Heilongjiang University), Ministry of Education, School of Chemistry and Materials Science, International Joint Research Center and Lab for Catalytic Technology, Harbin 150080, China
b.
School of Chemical and Environmental Engineering, Harbin University of Science and Technology, Harbin 150080, China

sunjh298@hlju.edu.cn

quyang@hlju.edu.cn

jinglq@hlju.edu.cn

Received Date: 12 June 2020
Revised Date: 28 June 2020
Accepted Date: 7 July 2020
Available Online: 17 July 2020

Figures(4)

Efficient generation of singlet oxygen (¹O₂) by an excitonic energy transfer process is highly desired on a semiconductor photocatalyst for selective oxidation of methyl phenyl sulfide (MPS). Herein, it is demonstrated that a large amount of ¹O₂ is produced on pristine graphitic carbon nitride (CN) nanosheet compared with bismuth oxybromide (BiOBr) and commercial P25 titanium dioxide (TiO₂). This leads to a certain photoactivity of CN for MPS oxidation. The observed ~77% selectivity for CN depends on the competitive results of excitonic energy transfer for ¹O₂ formation and charge carrier separation for superoxide radical (O₂^·-) production, which are based on the phosphorescence spectra and electron paramagnetic resonance signals, respectively. Moreover, ultrathin CN nanosheets are synthesized by thermal treatment with the cyanuric acid-melamine hydrogen bonded aggregates as precursors. It is confirmed that the amount of produced ¹O₂ could be increased by decreasing the thickness of resultant CN nanosheets. The optimized ultrathin CN nanosheet (~4 nm) exhibits excellent photoactivity with high selectivity (~99%). It is suggested that the excitonic energy transfer for ¹O₂ formation is close related to the intrinsic exciton binding energy and the two-dimensional quantum confinement effect. This work establishes a basic mechanistic understanding on the excitonic processes in CN, and develops a feasible route to design CN-based photocatalysts for efficient ¹O₂ generation.
- g-C₃N₄ nanosheet,
- Singlet oxygen generation,
- Excitonic energy transfer,
- Photocatalysis,
- Organic selective oxidation
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Efficient singlet oxygen generation by excitonic energy transfer on ultrathin g-C3N4 for selective photocatalytic oxidation of methyl-phenyl-sulfide with O2

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通讯作者: 陈斌, bchen63@163.com

Efficient singlet oxygen generation by excitonic energy transfer on ultrathin g-C₃N₄ for selective photocatalytic oxidation of methyl-phenyl-sulfide with O₂