Effect of Redox "Non-Innocent" Linker on the Catalytic Activity of Copper-Catecholate-Decorated Metal-Organic Frameworks

被引：50
作者：
Zhang, Xuan [1 ]
Vermeulen, Nicolaas A. [1 ]
Huang, Zhiyuan [2 ]
Cui, Yuexing [1 ]
Liu, Jian [1 ]
Krzyaniak, Matthew D. [1 ]
Li, Zhanyong [1 ]
Noh, Hyunho [1 ]
Wasielewski, Michael R. [1 ]
Delferro, Massimiliano [2 ]
Farha, Omar K. [1 ,3 ,4 ]
机构：
[1] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
[2] Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA
[3] Northwestern Univ, Dept Chem & Biol Engn, 2145 Sheridan Rd, Evanston, IL 60208 USA
[4] King Abdulaziz Univ, Dept Chem, Fac Sci, Jeddah 21589, Saudi Arabia
来源：
ACS APPLIED MATERIALS & INTERFACES | 2018年 / 10卷 / 01期
关键词：
redox-active; metal-organic frameworks; mixed-linker; catechol; copper catalyst; alkene oxidation; UiO-68; non-innocent; HETEROGENEOUS CATALYSTS; RETICULAR CHEMISTRY; OXIDATION; REDUCTION; LIGAND; CYCLOHEXENE; EPOXIDATION; POLYMERS; DESIGN; FILMS;
D O I：
10.1021/acsami.7b15326
中图分类号：
TB3 [工程材料学];
学科分类号：
0805 ; 080502 ;
摘要：
Two new UiO-68 type of Zr-MOFs featuring redox non-innocent catechol-based linkers of different redox activities have been synthesized through a de novo mixed-linker strategy. Metalation of the MOFs with Cu(II) precursors triggers the reduction of Cu(II) by the phenyl-catechol groups to Cu(I) with the concomitant formation of semiquinone radicals as evidenced by EPR and XPS characterization. The MOF-supported catalysts are selective toward the allylic oxidation of cyclohexene and it is found that the presence of in situ-generated Cu(I) species exhibits enhanced catalytic activity as compared to a similar MOF with Cu(II) metalated naphthalenyl-dihydroxy groups. This work unveils the importance of metal support redox interactions in the catalytic activity of MOF-supported catalysts which are not easily accessible in traditional metal oxide supports.
引用
收藏
页码：635 / 641
页数：7
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