Tuning Zr6 Metal–Organic Framework (MOF) Nodes as Catalyst Supports: Site Densities and Electron-Donor Properties Influence Molecular Iridium Complexes as Ethylene Conversion Catalysts

Yang, Dong; Odoh, Samuel O.; Borycz, Joshua; Wang, Timothy C.; Farha, Omar K.; Hupp, Joseph T.; Cramer, Christopher J.; Gagliardi, Laura; Gates, Bruce C.

doi:10.1021/acscatal.5b02243

Tuning Zr₆ Metal–Organic Framework (MOF) Nodes as Catalyst Supports: Site Densities and Electron-Donor Properties Influence Molecular Iridium Complexes as Ethylene Conversion Catalysts

Journal Article · Mon Nov 23 00:00:00 EST 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b02243· OSTI ID:1370933

Yang, Dong ^[1]; Odoh, Samuel O. ^[2]; Borycz, Joshua ^[2]; Wang, Timothy C. ^[3]; Farha, Omar K. ^[4]; Hupp, Joseph T. ^[3]; Cramer, Christopher J. ^[2]; Gagliardi, Laura ^[2]; Gates, Bruce C. ^[1]

Univ. of California, Davis, CA (United States)
Univ. of Minnesota, Minneapolis, MN (United States). Department of Chemistry, Chemical Theory Center, and Supercomputing Inst.
Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States); King Abdulaziz Univ., Jeddah (Saudi Arabia)

The Zr₆ nodes of the metal–organic frameworks (MOFs) UiO-66 and UiO-67 are metal oxide clusters of atomic precision and can be used as catalyst supports. The bonding sites on these nodes—that is, hydrogen-bonded H₂O/OH groups on UiO-67 and non-hydrogen-bonded terminal OH groups on UiO-66—were regulated by modulation of the MOF syntheses. Ir(C₂H₄)₂(C₅H₇O₂) complexes reacted with these sites to give site-isolated Ir(C₂H₄)₂ complexes, each anchored to the node by two Ir–Onode bonds. The supported iridium complexes on these sites have been characterized by infrared (IR) and extended X-ray absorption fine structure (EXAFS) spectroscopies and density functional theory calculations. The ethylene ligands on iridium are readily replaced by CO, and the ν_CO frequencies of the resultant complexes and those of comparable complexes reported elsewhere show that the support electron-donor tendencies increase in the order HY zeolite << UiO-66 < UiO-67 (= NU-1000) < ZrO₂ < MgO. The sharpness of the IR ν_CO bands shows that the degree of uniformity of the support bonding sites decreases in the order ZrO₂ ≈ UiO-67 ≈ NU-1000 < MgO < UiO-66 << HY zeolite. The reactivity of supported Ir(CO)₂ complexes with C2H4 to form Ir(C₂H₄)(CO) and Ir(C₂H₄)₂(CO) is influenced by the support electron-donor properties, with the reactivity increasing in the order MgO = ZrO₂ = NU-1000 (not reactive) < UiO-66 < UiO-67 << HY zeolite. Density functional theory calculations characterizing the complexes supported on NU-1000, UiO-66/67, and HY zeolite concur with the use of the calculated ν_CO bands as indicators of electron-donor properties of the supported metal catalysts. Our calculations also show that the reactivity of the supported Ir(CO)₂ complexes with C₂H₄ is correlated with the electron-donor properties of the iridium center. Lastly, the supported Ir(C₂H₄)₂ samples are precatalysts for ethylene hydrogenation and ethylene dimerization, with the activity for each reaction increasing with increasing electron-withdrawing strength of the support.

View Accepted Manuscript (DOE)

Research Organization:: 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) (SC-22)

Grant/Contract Number:: SC0012702

OSTI ID:: 1370933

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 1 Vol. 6; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalyst supports
ethylene dimerization
ethylene hydrogenation
iridium carbonyl complexes
iridium ethylene complexes
metal−organic framework nodes