Pd Nanoparticles Embedded into a Metal-Organic Framework: Synthesis, Structural Characteristics, and Hydrogen Sorption Properties

Zlotea, Claudia; Campesi, Renato; Cuevas, Fermín; Leroy, Éric; Dibandjo, Philippe; Volkringer, Christophe; Loiseau, Thierry; Férey, Gérard; Latroche, M.

doi:10.1021/ja9084995

Cited by 319 publications

(223 citation statements)

References 63 publications

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“…The synthesis of ultrasmall noble metal-based nanoparticles supported on a porous host is well documented due to extensive study of such materials for catalysis and hydrogen sorption (Campesi et al, 2008;Narehood et al, 2009;Zlotea et al, 2010a;Contescu et al, 2011). Typically, a metal salt is used as precursor for porous host impregnation followed by a reduction step (H2, NaBH4, etc.)…”

Section: Synthesismentioning

confidence: 99%

Experimental Challenges in Studying Hydrogen Absorption in Ultrasmall Metal Nanoparticles

et al. 2016

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Recent advances on synthesis, characterization, and hydrogen absorption properties of ultrasmall metal nanoparticles (defined here as objects with average size ≤3 nm) are briefly reviewed in the first part of this work. The experimental challenges encountered in performing accurate measurements of hydrogen absorption in Mg-and noble metal-based ultrasmall nanoparticles are addressed. The second part of this work reports original results obtained for ultrasmall bulk-immiscible Pd-Rh nanoparticles. Carbonsupported Pd-Rh nanoalloys in the whole binary chemical composition range have been successfully prepared by liquid impregnation method followed by reduction at 300°C. EXAFS investigations suggested that the local structure of these nanoalloys is partially segregated into Rh-rich core and Pd-rich surface coexisting within the same nanoparticles. Downsizing to ultrasmall dimensions completely suppresses the hydride formation in Pd-rich nanoalloys at ambient conditions, contrary to bulk and larger nanosized (5-6 nm) counterparts. The ultrasmall Pd90Rh10 nanoalloy can absorb hydrogen-forming solid solutions under these conditions, as suggested by in situ X-ray diffraction (XRD). Apart from this composition, common laboratory techniques, such as in situ XRD, DSC, and PCI, failed to clarify the hydrogen interaction mechanism: either adsorption on developed surfaces or both adsorption and absorption with formation of solid solutions. Concluding insights were brought by in situ EXAFS experiments at synchrotron: ultrasmall Pd75Rh25 and Pd50Rh50 nanoalloys absorb hydrogen-forming solid solutions at ambient conditions. Moreover, the hydrogen solubility in these solid solutions is higher with increasing Pd content, and this trend can be understood in terms of hydrogen preferential occupation in the Pd-rich regions, as suggested by in situ EXAFS. The Rh-rich nanoalloys (Pd25Rh75 and Pd10Rh90) only adsorb hydrogen on the developed surface of ultrasmall nanoparticles. In summary, in situ characterization techniques carried out at large-scale facilities are unique and powerful tools for in-depth investigation of hydrogen interaction with ultrasmall nanoparticles at local level.

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Section: Synthesismentioning

confidence: 99%

Experimental Challenges in Studying Hydrogen Absorption in Ultrasmall Metal Nanoparticles

et al. 2016

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“…MOFs [1][2][3][4][5][6][7][8] are very attractive due to the possibility of designing a structure with a particular pore size and shape from multifunctional ligands and metal ions. MOFs have been widely studied in the field of gas storage, [9][10][11][12][13] catalysis, [14][15][16][17] removal of harmful materials, [18,19] separation, [20][21][22] magnetism, [23,24] carrier of nano-materials, [25,26] and drug delivery. [27,28] So far, the major studies on MOFs have been the syntheses, structure analyses, and potential applications in various fields.…”

Section: Introductionmentioning

confidence: 99%

Chemical and Thermal Stability of Isotypic Metal–Organic Frameworks: Effect of Metal Ions

Kang

Khan

Haque

et al. 2011

Chemistry A European J

271

174

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Chemical and thermal stabilities of isotypic metal-organic frameworks (MOFs) like Al-BDC (Al-benzenedicarboxylate called MIL-53-Al), Cr-BDC (MIL-53-Cr) and V-BDC (MIL-47-V), after purification to remove uncoordinated organic linkers, have been compared to understand the effect of the central metal ions on the stabilities of the porous MOF-type materials. Chemical stability to acids, bases, and water decreases in the order of Cr-BDC>Al-BDC>V-BDC, suggesting stability increases with increasing inertness of the central metal ions. However, thermal stability decreases in the order of Al-BDC>Cr-BDC> V-BDC, and this tendency may be explained by the strength of the metal-oxygen bond in common oxides like Al(2)O(3), Cr(2)O(3), and V(2)O(5). In order to evaluate precisely the stability of a MOF, it is necessary to remove uncoordinated organic linkers that are located in the pores of the MOF, because a filled MOF may be more stable than the same MOF after purification.

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“…Various applications of MOFs, such as gas storage [30][31][32] and separation [33,34], have been studied. Applications of MOFs in catalysis have also been explored [35][36][37][38][39][40][41][42][43][44][45][46][47].…”

Section: Introductionmentioning

confidence: 99%

Synthesis of cyclic carbonates and dimethyl carbonate using CO2 as a building block catalyzed by MOF-5/KI and MOF-5/KI/K2CO3

et al. 2011

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The synthesis of cyclic carbonates or dimethyl carbonate (DMC) using CO 2 as a building block is a very interesting topic. In this work, we found that the metalorganic framework-5 (MOF-5)/KI was an active and a selective catalytic system for the synthesis of cyclic carbonates from CO 2 and epoxides, and MOF-5/KI/ K 2 CO 3 was efficient for the preparation of DMC from CO 2 , propylene, and methanol by a sequential route. The impacts of temperature, pressure, and reaction time length on the reactions were investigated, and the mechanism of the reactions is proposed on the basis of the experimental results.

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Pd Nanoparticles Embedded into a Metal-Organic Framework: Synthesis, Structural Characteristics, and Hydrogen Sorption Properties

Cited by 319 publications

References 63 publications

Experimental Challenges in Studying Hydrogen Absorption in Ultrasmall Metal Nanoparticles

Experimental Challenges in Studying Hydrogen Absorption in Ultrasmall Metal Nanoparticles

Chemical and Thermal Stability of Isotypic Metal–Organic Frameworks: Effect of Metal Ions

Synthesis of cyclic carbonates and dimethyl carbonate using CO2 as a building block catalyzed by MOF-5/KI and MOF-5/KI/K2CO3

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