Hydrogen Absorption In 1 Nm Pd Clusters Confined In MIL-101(Cr)

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From the journal:

Journal of Materials Chemistry A

Hydrogen absorption in 1 nm Pd clusters confined in MIL-101(Cr)†

Abdelmalek Malouche,a Gabriela Blanita,b Dan Lupu,b Julie Bourgon,a Jaysen Nelayahc and Claudia Zlotea *a Author affiliations

* Corresponding authors

a Université Paris Est, Institut de Chimie et des Matériaux Paris-Est (UMR7182), CNRS, UPEC, 2-8 rue Henri Dunant, F-94320 Thiais, France E-mail: [email protected]

b National Institute for Research and Development of Isotopic and Molecular Technologies, 67-103 Donat Str., RO-400293 Cluj-Napoca, Romania

c Université Paris Diderot, Sorbonne Paris Cité, CNRS, Laboratoire Matériaux et Phénomènes Quantiques, UMR 7162, Paris, France

Abstract

We report here the unprecedented modification of the hydrogen absorption/desorption properties of 1 nm Pd clusters relative to the bulk and nanoparticles down to 2–3 nm. These metal clusters have been synthesized by a facile double solvent impregnation method. They contain on average 33 atoms and are confined/stabilized into a metal-organic-framework with different metal loadings (5–20 wt%). This is the first time, to the best of our knowledge, that 1 nm Pd clusters are effectively confined into a MOF for high metal loadings. Such ultra-small nanoparticles are crystalline with the archetypical fcc structure of the bulk metal, as confirmed by both HR-TEM and in situ EXAFS. Hydrogen absorption/desorption properties of 1 nm Pd clusters have been characterized by both laboratory and synchrotron facilities. Under ambient conditions, 1 nm Pd clusters absorb hydrogen forming solid solutions instead of a hydride phase, as usually encountered for the bulk and Pd nanoparticles down to 2–3 nm. This can be understood by a decrease of the critical temperature of the two-phase region in the Pd–H phase diagram below room temperature. Moreover, the activation energy of hydrogen desorption from Pd clusters strongly decreases relative to bulk Pd. This suggests a change in the rate limiting step from surface recombination or β → α phase transformation usually encountered in bulk Pd to hydrogen diffusion into α and β phases in 1 nm clusters.

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Article information

DOI https://doi.org/10.1039/C7TA07159K Article type Paper Submitted 14 Aug 2017 Accepted 09 Oct 2017 First published 10 Oct 2017

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J. Mater. Chem. A, 2017,5, 23043-23052 BibTex EndNote MEDLINE ProCite ReferenceManager RefWorks RIS

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Hydrogen absorption in 1 nm Pd clusters confined in MIL-101(Cr)

A. Malouche, G. Blanita, D. Lupu, J. Bourgon, J. Nelayah and C. Zlotea, J. Mater. Chem. A, 2017, 5, 23043 DOI: 10.1039/C7TA07159K

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Abdelmalek Malouche Gabriela Blanita Dan Lupu Julie Bourgon Jaysen Nelayah Claudia Zlotea

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