Confined Cu Single Sites in ZSM-5 for Photocatalytic Hydroxylation of Benzene to Phenol

被引:1
|
作者
Zhang, Jinwen [1 ,2 ]
Ding, Hongxin [1 ,2 ]
Hui, Hehua [1 ,2 ]
Yao, Qingying [1 ,2 ]
Feng, Wenhua [1 ,2 ]
Chen, Tian-xiang [3 ]
Lo, Tsz Woon Benedict [3 ]
Ren, Yuanhang [1 ,2 ]
Ye, Lin [1 ,2 ]
Yue, Bin [1 ,2 ]
He, Heyong [1 ,2 ]
机构
[1] Fudan Univ, Dept Chem, Shanghai 200438, Peoples R China
[2] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China
[3] Hong Kong Polytech Univ, Dept Appl Biol & Chem Technol, Hong Kong 999077, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
benzene hydroxylation; heterogeneous catalysis; photocatalysis; single atom Cu@ZSM-5; ultra-wide bandgap; SELECTIVE OXIDATION; CARBON NITRIDE; NANOPARTICLES; MOLECULES; CATALYSTS; ZEOLITE; ACIDITY; OXIDES; TIO2;
D O I
10.1002/smll.202405150
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Zeolites with band-like charge transport properties have exhibited their potential activities in sensing, optics, and electronics. Herein, a precisely designed Cu@ZSM-5 catalyst is presented with an ultra-wide bandgap of 4.27 eV, showing excellent photocatalytic activity in hydroxylation of benzene with benzene conversion 27.9% and phenol selectivity 97.6%. The SXRD and Rietveld refinement results illustrate that Cu@ZSM-5 has an average of 0.8 Cu atoms per unit cell and the single Cu atoms located in the cross-section of the sinusoidal and straight channels. XANES and EXAFS further demonstrate that the Cu atoms have an oxidation state of +2, coordinated with three OMFI-framework atoms and one & horbar;OH group. Detailed characterizations demonstrate that the Cu@ZSM-5 with tailored bandgap is able to enhance the photoinduced electron-hole separation and hence promote selective hydroxylation of benzene to phenol via the superoxide radical route. This work may open a new way for designing electrically conductive zeolite-supported photocatalysts. Herein, a precisely fabricated Cu@ZSM-5 catalyst with single [Cu(OH)]+ species anchored in a specific position of the ZSM-5 framework exhibits a competitive photocatalytic activity in benzene hydroxylation to phenol. This work provides a new strategy for designing conductive catalysts in photocatalytic catalysis. image
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页数:8
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