Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption

Palladium nanoparticles can split the dihydrogen bond and produce atomic hydrogen. When the metal nanoparticles are in intimate contact with a hydrogen-atom host, chemisorption of H-atoms by the host has been suggested to occur via the hydrogen spillover mechanism. Metal–organic frameworks were pred...

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Main Authors: Szilagyi, Petra, Callini, E., Anastasopol, A., Kwakernaak, C., Sachdeva, S., van de Krol, R., Geerlings, H., Borgschulte, A., Zuttel, A., Dam, B.
Format: Journal Article
Published: R S C Publications 2014
Online Access:http://pubs.rsc.org/en/content/articlepdf/2014/cp/c3cp54898h
http://hdl.handle.net/20.500.11937/49465
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author Szilagyi, Petra
Callini, E.
Anastasopol, A.
Kwakernaak, C.
Sachdeva, S.
van de Krol, R.
Geerlings, H.
Borgschulte, A.
Zuttel, A.
Dam, B.
author_facet Szilagyi, Petra
Callini, E.
Anastasopol, A.
Kwakernaak, C.
Sachdeva, S.
van de Krol, R.
Geerlings, H.
Borgschulte, A.
Zuttel, A.
Dam, B.
author_sort Szilagyi, Petra
building Curtin Institutional Repository
collection Online Access
description Palladium nanoparticles can split the dihydrogen bond and produce atomic hydrogen. When the metal nanoparticles are in intimate contact with a hydrogen-atom host, chemisorption of H-atoms by the host has been suggested to occur via the hydrogen spillover mechanism. Metal–organic frameworks were predicted to be able to act as effective chemisorption sites, and increased ambient-temperature hydrogen adsorption was reported on several occasions. The intimate contact was supposedly ensured by the use of a carbon bridge. In this work, we show that it is possible to introduce catalyst palladium particles into MOF’s pores and simultaneously ensuring good contact, making the employment of the carbon bridge redundant. The addition of Pd nanoparticles indeed increases the ambient-temperaturehydrogen uptake of the framework, but this is found to be solely due to palladium hydride formation. In addition, we show that the hydrogen atoms do not chemisorb on the host framework, which excludes the possibility of hydrogen spillover.
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format Journal Article
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institution Curtin University Malaysia
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last_indexed 2025-11-14T09:40:55Z
publishDate 2014
publisher R S C Publications
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spelling curtin-20.500.11937-494652017-03-15T22:56:20Z Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption Szilagyi, Petra Callini, E. Anastasopol, A. Kwakernaak, C. Sachdeva, S. van de Krol, R. Geerlings, H. Borgschulte, A. Zuttel, A. Dam, B. Palladium nanoparticles can split the dihydrogen bond and produce atomic hydrogen. When the metal nanoparticles are in intimate contact with a hydrogen-atom host, chemisorption of H-atoms by the host has been suggested to occur via the hydrogen spillover mechanism. Metal–organic frameworks were predicted to be able to act as effective chemisorption sites, and increased ambient-temperature hydrogen adsorption was reported on several occasions. The intimate contact was supposedly ensured by the use of a carbon bridge. In this work, we show that it is possible to introduce catalyst palladium particles into MOF’s pores and simultaneously ensuring good contact, making the employment of the carbon bridge redundant. The addition of Pd nanoparticles indeed increases the ambient-temperaturehydrogen uptake of the framework, but this is found to be solely due to palladium hydride formation. In addition, we show that the hydrogen atoms do not chemisorb on the host framework, which excludes the possibility of hydrogen spillover. 2014 Journal Article http://hdl.handle.net/20.500.11937/49465 http://pubs.rsc.org/en/content/articlepdf/2014/cp/c3cp54898h R S C Publications restricted
spellingShingle Szilagyi, Petra
Callini, E.
Anastasopol, A.
Kwakernaak, C.
Sachdeva, S.
van de Krol, R.
Geerlings, H.
Borgschulte, A.
Zuttel, A.
Dam, B.
Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption
title Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption
title_full Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption
title_fullStr Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption
title_full_unstemmed Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption
title_short Probing hydrogen spillover in Pd@MIL-101(Cr) with a focus on hydrogen chemisorption
title_sort probing hydrogen spillover in pd@mil-101(cr) with a focus on hydrogen chemisorption
url http://pubs.rsc.org/en/content/articlepdf/2014/cp/c3cp54898h
http://hdl.handle.net/20.500.11937/49465