期刊
ACS APPLIED MATERIALS & INTERFACES
卷 10, 期 1, 页码 635-641出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b15326
关键词
redox-active; metal-organic frameworks; mixed-linker; catechol; copper catalyst; alkene oxidation; UiO-68; non-innocent
资金
- U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) [DESC0012702]
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, DOE [DE-FG02-99ER14999]
- U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
- MRSEC program at the Materials Research Center [NSF DMR-1121262]
- International Institute for Nanotechnology (IIN)
- Keck Foundation
- State of Illinois, through the IIN
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.
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