Covalent combination of polyoxometalate and graphitic carbon nitride for light-driven hydrogen peroxide production

被引:175
作者
Zhao, Shen [1 ]
Zhao, Xu [1 ]
Zhang, Hui [2 ]
Li, Jiang [1 ]
Zhu, Yongfa [3 ]
机构
[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Key Lab Drinking Water Sci & Technol, Beijing 100085, Peoples R China
[2] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China
[3] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
关键词
Graphitic carbon nitride; Polyoxometalates; Covalent combination; Hydrogen peroxide production; PHOTOCATALYTIC H2O2 PRODUCTION; WATER OXIDATION CATALYSTS; METAL-FREE PHOTOCATALYSTS; VISIBLE-LIGHT; EFFICIENT PHOTOCATALYST; MOLECULAR-OXYGEN; PHOTOREDOX CATALYSIS; ENERGY-CONVERSION; FUEL; GENERATION;
D O I
10.1016/j.nanoen.2017.04.017
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
The polyoxometalate (POM) cluster of [PW11O39](7-) (PW11) has been successfully covalent combined with the three dimensionally ordered macroporous graphitic carbon nitride (3DOM g-C3N4) through the organic linker strategy. The characterization such as solid-state NMR and XPS results confirm the organosilicon agent of (triethoxysilyl)-propyl isocyanate can act as the linker to covalent combine the PW11 cluster with 3DOM g-C3N4. The hybrid catalyst of 3DOM g-C3N4-PW11 exhibits efficient catalytic performance (2.4 mu mol h(-1)) for light-driven H2O2 production from H2O and O-2 in the absence of organic electron donors. The ESR results suggest that one-electron reduction of O-2 to center dot OOH is indeed suppressed over 3DOM g-C3N4-PW11. Furthermore, the Koutecky-Levich plot obtained from electrochemical rotating disk electrode (RDE) analysis of oxygen reduction reaction (ORR) for 3DOM g-C3N4-PW11 reveals the value of electron transfer during the ORR process is 2.30, indicating the covalent combination can promote the two-electron O-2 reduction. In addition, the recycle experiment results reveal that the heterogeneous 3DOM g-C3N4-PW11 is catalytic stable.
引用
收藏
页码:405 / 414
页数:10
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