Cargando…

Revealing hydrogen spillover pathways in reducible metal oxides

Hydrogen spillover, the migration of dissociated hydrogen atoms from noble metals to their support materials, is a ubiquitous phenomenon and is widely utilized in heterogeneous catalysis and hydrogen storage materials. However, in-depth understanding of the migration of spilled hydrogen over differe...

Descripción completa

Detalles Bibliográficos
Autores principales: Shun, Kazuki, Mori, Kohsuke, Masuda, Shinya, Hashimoto, Naoki, Hinuma, Yoyo, Kobayashi, Hisayoshi, Yamashita, Hiromi
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9278487/
https://www.ncbi.nlm.nih.gov/pubmed/35919430
http://dx.doi.org/10.1039/d2sc00871h
_version_ 1784746197388361728
author Shun, Kazuki
Mori, Kohsuke
Masuda, Shinya
Hashimoto, Naoki
Hinuma, Yoyo
Kobayashi, Hisayoshi
Yamashita, Hiromi
author_facet Shun, Kazuki
Mori, Kohsuke
Masuda, Shinya
Hashimoto, Naoki
Hinuma, Yoyo
Kobayashi, Hisayoshi
Yamashita, Hiromi
author_sort Shun, Kazuki
collection PubMed
description Hydrogen spillover, the migration of dissociated hydrogen atoms from noble metals to their support materials, is a ubiquitous phenomenon and is widely utilized in heterogeneous catalysis and hydrogen storage materials. However, in-depth understanding of the migration of spilled hydrogen over different types of supports is still lacking. Herein, hydrogen spillover in typical reducible metal oxides, such as TiO(2), CeO(2), and WO(3), was elucidated by combining systematic characterization methods involving various in situ techniques, kinetic analysis, and density functional theory calculations. TiO(2) and CeO(2) were proven to be promising platforms for the synthesis of non-equilibrium RuNi binary solid solution alloy nanoparticles displaying a synergistic promotional effect in the hydrolysis of ammonia borane. Such behaviour was driven by the simultaneous reduction of both metal cations under a H(2) atmosphere over TiO(2) and CeO(2), in which hydrogen spillover favorably occurred over their surfaces rather than within their bulk phases. Conversely, hydrogen atoms were found to preferentially migrate within the bulk prior to the surface over WO(3). Thus, the reductions of both metal cations occurred individually on WO(3), which resulted in the formation of segregated NPs with no activity enhancement.
format Online
Article
Text
id pubmed-9278487
institution National Center for Biotechnology Information
language English
publishDate 2022
publisher The Royal Society of Chemistry
record_format MEDLINE/PubMed
spelling pubmed-92784872022-08-01 Revealing hydrogen spillover pathways in reducible metal oxides Shun, Kazuki Mori, Kohsuke Masuda, Shinya Hashimoto, Naoki Hinuma, Yoyo Kobayashi, Hisayoshi Yamashita, Hiromi Chem Sci Chemistry Hydrogen spillover, the migration of dissociated hydrogen atoms from noble metals to their support materials, is a ubiquitous phenomenon and is widely utilized in heterogeneous catalysis and hydrogen storage materials. However, in-depth understanding of the migration of spilled hydrogen over different types of supports is still lacking. Herein, hydrogen spillover in typical reducible metal oxides, such as TiO(2), CeO(2), and WO(3), was elucidated by combining systematic characterization methods involving various in situ techniques, kinetic analysis, and density functional theory calculations. TiO(2) and CeO(2) were proven to be promising platforms for the synthesis of non-equilibrium RuNi binary solid solution alloy nanoparticles displaying a synergistic promotional effect in the hydrolysis of ammonia borane. Such behaviour was driven by the simultaneous reduction of both metal cations under a H(2) atmosphere over TiO(2) and CeO(2), in which hydrogen spillover favorably occurred over their surfaces rather than within their bulk phases. Conversely, hydrogen atoms were found to preferentially migrate within the bulk prior to the surface over WO(3). Thus, the reductions of both metal cations occurred individually on WO(3), which resulted in the formation of segregated NPs with no activity enhancement. The Royal Society of Chemistry 2022-06-24 /pmc/articles/PMC9278487/ /pubmed/35919430 http://dx.doi.org/10.1039/d2sc00871h Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Shun, Kazuki
Mori, Kohsuke
Masuda, Shinya
Hashimoto, Naoki
Hinuma, Yoyo
Kobayashi, Hisayoshi
Yamashita, Hiromi
Revealing hydrogen spillover pathways in reducible metal oxides
title Revealing hydrogen spillover pathways in reducible metal oxides
title_full Revealing hydrogen spillover pathways in reducible metal oxides
title_fullStr Revealing hydrogen spillover pathways in reducible metal oxides
title_full_unstemmed Revealing hydrogen spillover pathways in reducible metal oxides
title_short Revealing hydrogen spillover pathways in reducible metal oxides
title_sort revealing hydrogen spillover pathways in reducible metal oxides
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9278487/
https://www.ncbi.nlm.nih.gov/pubmed/35919430
http://dx.doi.org/10.1039/d2sc00871h
work_keys_str_mv AT shunkazuki revealinghydrogenspilloverpathwaysinreduciblemetaloxides
AT morikohsuke revealinghydrogenspilloverpathwaysinreduciblemetaloxides
AT masudashinya revealinghydrogenspilloverpathwaysinreduciblemetaloxides
AT hashimotonaoki revealinghydrogenspilloverpathwaysinreduciblemetaloxides
AT hinumayoyo revealinghydrogenspilloverpathwaysinreduciblemetaloxides
AT kobayashihisayoshi revealinghydrogenspilloverpathwaysinreduciblemetaloxides
AT yamashitahiromi revealinghydrogenspilloverpathwaysinreduciblemetaloxides