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Hydrogen Storage in New Metal–Organic Frameworks
Tranchemontagne, David J.,Park, Kyo Sung,Furukawa, Hiroyasu,Eckert, Juergen,Knobler, Carolyn B.,Yaghi, Omar M. American Chemical Society 2012 The Journal of Physical Chemistry Part C Vol.116 No.24
<P>Five new metal–organic frameworks (MOFs, termed MOF-324, 325, 326 and IRMOF-61 and 62) of either short linkers (pyrazolecarboxylate and pyrazaboledicarboxylate) or long and thin alkyne functionalities (ethynyldibenzoate and butadiynedibenzoate) were prepared to examine their impact on hydrogen storage in MOFs. These compounds were characterized by single-crystal X-ray diffraction, and their low-pressure and high-pressure hydrogen uptake properties were investigated. In particular, volumetric excess H<SUB>2</SUB> uptake by MOF-324 and IRMOF-62 outperforms MOF-177 up to 30 bar. Inelastic neutron-scattering studies for MOF-324 also revealed strong interactions between the organic links and hydrogen, in contrast to MOF-5 where the interactions between the Zn<SUB>4</SUB>O unit and hydrogen are the strongest. These data also show that smaller pores and polarized linkers in MOFs are indeed advantageous for hydrogen storage.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpccck/2012/jpccck.2012.116.issue-24/jp302356q/production/images/medium/jp-2012-02356q_0008.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/jp302356q'>ACS Electronic Supporting Info</A></P>
Metal–Organic Frameworks of Vanadium as Catalysts for Conversion of Methane to Acetic Acid
Phan, Anh,Czaja, Alexander U.,Gá,ndara, Felipe,Knobler, Carolyn B.,Yaghi, Omar M. American Chemical Society 2011 Inorganic chemistry Vol.50 No.16
<P>A catalytic system combining the high activity of homogeneous catalysts and the ease of use of heterogeneous catalysts for methane activation is reported. The vanadium-containing metal–organic frameworks (MOFs) MIL-47 and MOF-48 are found to have high catalytic activity and chemical stability. They convert methane selectively to acetic acid with 70% yield (490 TON) based on K<SUB>2</SUB>S<SUB>2</SUB>O<SUB>8</SUB> as an oxidant. Isotopic labeling experiments showed that two methane molecules are converted to the produced acetic acid. The MOF catalysts are reusable and remain catalytically active for several recycling steps without losing their crystalline structures.</P><P>The vanadium-containing metal−organic framework MOF-48 catalyzes the selective direct oxidation of methane to acetic acid. The yield is 49% (based on K<SUB>2</SUB>S<SUB>2</SUB>O<SUB>8</SUB> as an oxidant), 490 TON, at 80 °C in a trifluoroacetic acid solvent.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/inocaj/2011/inocaj.2011.50.issue-16/ic201396m/production/images/medium/ic-2011-01396m_0005.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ic201396m'>ACS Electronic Supporting Info</A></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ic201396m'>ACS Electronic Supporting Info</A></P>