Title
Pd@MOF-5: limitations of gas-phase infiltration and solution impregnation of <tex>$[Zn_{4}O(bdc)_{3}]$</tex> (MOF-5) with metalorganic palladium precursors for loading with Pd nanoparticles Pd@MOF-5: limitations of gas-phase infiltration and solution impregnation of <tex>$[Zn_{4}O(bdc)_{3}]$</tex> (MOF-5) with metalorganic palladium precursors for loading with Pd nanoparticles
Author
Faculty/Department
Faculty of Sciences. Physics
Publication type
article
Publication
Cambridge ,
Subject
Physics
Chemistry
Source (journal)
Journal of materials chemistry / Royal Society of Chemistry. - Cambridge, 1991 - 2012
Volume/pages
19(2009) :9 , p. 1314-1319
ISSN
0959-9428
1364-5501
ISI
000263450300015
Carrier
E
Target language
English (eng)
Full text (Publishers DOI)
Affiliation
University of Antwerp
Abstract
The limitations of the loading of the porous metalorganic framework [Zn4O(bdc)3] (bdc = benzene-1,4-dicarboxylate; MOF-5 or IRMOF-1) with Pd nanoparticles was investigated. First, the volatile organometallic precursor [Pd(5-C5H5)(3-C3H5)] was employed to get the inclusion compound [Pd(5-C5H5)(3-C3H5)]x@MOF-5 via gas-phase infiltration at 10-3 mbar. A loading of four molecules of [Pd(5-C5H5)(3-C3H5)] per formula unit of MOF-5 (x = 4) can be reached (35 wt.% Pd). Second, the metalorganic precursor [Pd(acac)2] (acac = 2,4-pentanedionate) was used and the inclusion materials [Pd(acac)2]x@MOF-5 of different Pd loadings were obtained by incipient wetness infiltration. However, the maximum loading was lower as compared with the former case with about two precursor molecules per formula unit of MOF-5. Both loading routes are suitable for the synthesis of Pd nanoparticles inside the porous host matrix. Homogeneously distributed nanoparticles with diameter of 2.4(±0.2) nm can be achieved by photolysis of the inclusion compounds [Pd(5-C5H5)(3-C3H5)]x@MOF-5 (x 4), while the hydrogenolysis of [Pd(acac)2]x@MOF-5 (x 2) leads to a mixture of small particles inside the network (< 3 nm) and large Pd agglomerates (40 nm) on the outer surface of the MOF-5 specimens. The pure Pdx@MOF-5 materials proved to be stable under hydrogen pressure (2 bar) at 150 °C over many hours. Neither hydrogenation of the bdc linkers nor particle growth was observed. The new composite materials were characterized by 1H/13C-MAS-NMR, powder XRD, ICP-AES, FT-IR, N2 sorption measurements and high resolution TEM. Raising the Pd loading of a representative sample Pd4@MOF-5 (35 wt.% Pd) by using [Pd(5-C5H5)(3-C3H5)] as precursor in a second cycle of gas-phase infiltration and photolysis was accompanied by the collapse of the long-range crystalline order of the MOF.
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