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

Zhang, Xuan; Vermeulen, Nicolaas A.; Huang, Zhiyuan; Cui, Yuexing; Liu, Jian; Krzyaniak, Matthew D.; Li, Zhanyong; Noh, Hyunho; Wasielewski, Michael R.; Delferro, Massimiliano; Farha, Omar K.

doi:10.1021/acsami.7b15326

Title: Effect of Redox “Non-Innocent” Linker on the Catalytic Activity of Copper-Catecholate-Decorated Metal–Organic Frameworks

Journal Article · Tue Dec 26 00:00:00 EST 2017 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b15326· OSTI ID:1421963

^[1]; Vermeulen, Nicolaas A. ^[2]; Huang, Zhiyuan ^[3]; Cui, Yuexing ^[2]; Liu, Jian ^[2]; Krzyaniak, Matthew D. ^[2];

^[2]; Noh, Hyunho ^[2];

^[2];

^[3];

^[4]

Northwestern Univ., Evanston, IL (United States). Department of Chemistry
Northwestern Univ., Evanston, IL (United States). Department of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences & Engineering Division
Northwestern Univ., Evanston, IL (United States). Department of Chemistry and Department of Chemical and Biological Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences & Engineering Division; King Abdulaziz Univ., Jeddah (Saudi Arabia). Department of Chemistry, Faculty of Science

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. Also, 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. Here, 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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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF); Northwestern University - International Institute for Nanotechnology (IIN)

Grant/Contract Number:: AC02-06CH11357; SC0012702; FG02-99ER14999

OSTI ID:: 1421963

Journal Information:: ACS Applied Materials and Interfaces, Vol. 10, Issue 1; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 40 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alkene oxidation
catechol
copper catalyst
metal−organic frameworks
mixed-linker
non-innocent
redox-active
UiO-68

Title: Effect of Redox “Non-Innocent” Linker on the Catalytic Activity of Copper-Catecholate-Decorated Metal–Organic Frameworks

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