Further Investigation of the Effect of Framework Catenation on Hydrogen Uptake in Metal--Organic Frameworks.
Hydrogen-sorption studies have been carried out for the catenation isomer pairs of PCN-6 and PCN-6′ (both have the formula of Cu(TATB), where TATB represents 4,4′,4″-s-triazine-2,4,6-triyltribenzoate with a formula of CHNO). Inelastic neutron scattering (INS) studies reveal that the initial sites oc...
| Publicado en: | Journal of the American Chemical Society Vol. 130; no. 47; pp. 15896 - 15903 |
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| Autores principales: | , , , , , , , , |
| Formato: | Artículo |
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American Chemical Society
11/26/2008
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=35614361&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 35614361 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 11/26/2008 vid: 130 iid: 47 pid: 997 pub: American Chemical Society artinfo: ui: 35614361 10.1021/ja803492q ppf: 15896 ppct: 7 formats: tig: atl: Further Investigation of the Effect of Framework Catenation on Hydrogen Uptake in Metal--Organic Frameworks. aug: au: Shengqian Ma Eckert, Juergen Forster, Paul M. Ji Woong Yoon Young Kyu Hwang Jong-San Chang Collier, Christopher D. Parise, John B. Hong-Cai Zhou affil: Department of Chemistry, Texas A&M University, P.O. Box 30012, College Station, Texas 77842-3012 Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Avenue, Argonne, IL 60439 Materials Research Laboratory, University of California, Santa Barbara, California 93106 Department for Chemistry, University of Nevada, Las Vegas, Nevada 89154 Catalysis Center for Molecular Engineering, Korea Research Institute of Chemical Technology (KRICT), Jang-dong 100, Yuseong-Gu, daejon 305-600, Korea Mineral Physics Institute, Stony Brook University, Stony Brook, New York 11794 su: Hydrogen spectra Absorption Separation (Technology) Surface chemistry Structural frames Structural analysis (Engineering) sug: subj: Hydrogen spectra Absorption Separation (Technology) Surface chemistry Structural frames Structural analysis (Engineering) ab: Hydrogen-sorption studies have been carried out for the catenation isomer pairs of PCN-6 and PCN-6′ (both have the formula of Cu(TATB), where TATB represents 4,4′,4″-s-triazine-2,4,6-triyltribenzoate with a formula of CHNO). Inelastic neutron scattering (INS) studies reveal that the initial sites occupied by adsorbed H are the open Cu centers of the paddlewheel units with comparable interaction energies in the two isomers. At high H loadings, where the H molecules adsorb mainly on or around the organic linkers, the interaction is found to be substantially stronger in catenated PCN-6 than in noncatenated PCN-6′, leading to much higher H uptake in the isomer with catenation. Hydrogen sorption measurements at pressures up to 50 bar demonstrate that framework catenation can be favorable for the enhancement of hydrogen adsorption. For example, the excess hydrogen uptake of PCN-6 is 72 mg/g (6.7 wt %) at 77 K/50 bar or 9.3 mg/g (0.92 wt %) at 298 K/50 bar, respectively, and that for PCN-6′ is 42 mg/g (4.0 wt %) at 77 K/50 bar or 4.0 mg/g (0.40 wt %) at 298 K/50 bar. Importantly, PCN-6 exhibits a total hydrogen uptake of 95 mg/g (8.7 wt %) (corresponding to a total volumetric value of 53.0 g/L, estimated based on crystallographic density) at 77 K/50 bar and 15 mg/g (1.5 wt %) at 298 K/50 bar. Significantly, the expected usable capacity of PCN-6 is as high as 75 mg/g (or 41.9 g/L) at 77 K, if a recharging pressure of 1.5 bar is assumed. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2008 holdings: @attributes: islocal: N |
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