Dispersed surface Ru ensembles on MgO(111) for catalytic ammonia decomposition

Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO supp...

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Published inNature communications Vol. 14; no. 1; pp. 647 - 15
Main Authors Fang, Huihuang, Wu, Simson, Ayvali, Tugce, Zheng, Jianwei, Fellowes, Joshua, Ho, Ping-Luen, Leung, Kwan Chee, Large, Alexander, Held, Georg, Kato, Ryuichi, Suenaga, Kazu, Reyes, Yves Ira A., Thang, Ho Viet, Chen, Hsin-Yi Tiffany, Tsang, Shik Chi Edman
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 06.02.2023
Nature Publishing Group
Nature Portfolio
Subjects
119/118
147/137
639/301/299
639/4077/4079/4088/4089
639/638/77/887
Ammonia
Bimetals
Catalysts
Clusters
Decomposition
Dehydrogenation
Dispersion
Humanities and Social Sciences
Hydrogen storage
Magnesium oxide
Metals
multidisciplinary
Nanoparticles
Renewable energy
Ruthenium
Science
Science (multidisciplinary)
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Abstract Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N 2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N 2 /H 2 , as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B 5 sites) than isolated sites. Ruthenium-based materials show promising performance for ammonia decomposition, yet the underlying mechanism remains to be further explored. Here the authors investigate atomically dispersed Ru atoms on polar (111) on MgO facets to show synergistic metal sites in close proximity are required for the stepwise dehydrogenation of ammonia to N2/H2.
AbstractList Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N2/H2, as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B5 sites) than isolated sites.Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N2/H2, as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B5 sites) than isolated sites.
Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N complexes in solution are required for the stepwise dehydrogenation of ammonia to N /H , as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B sites) than isolated sites.
Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N 2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N 2 /H 2 , as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B 5 sites) than isolated sites. Ruthenium-based materials show promising performance for ammonia decomposition, yet the underlying mechanism remains to be further explored. Here the authors investigate atomically dispersed Ru atoms on polar (111) on MgO facets to show synergistic metal sites in close proximity are required for the stepwise dehydrogenation of ammonia to N2/H2.
Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N 2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N 2 /H 2 , as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B 5 sites) than isolated sites.
Ruthenium-based materials show promising performance for ammonia decomposition, yet the underlying mechanism remains to be further explored. Here the authors investigate atomically dispersed Ru atoms on polar (111) on MgO facets to show synergistic metal sites in close proximity are required for the stepwise dehydrogenation of ammonia to N2/H2.
Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N2/H2, as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B5 sites) than isolated sites.Ruthenium-based materials show promising performance for ammonia decomposition, yet the underlying mechanism remains to be further explored. Here the authors investigate atomically dispersed Ru atoms on polar (111) on MgO facets to show synergistic metal sites in close proximity are required for the stepwise dehydrogenation of ammonia to N2/H2.
ArticleNumber 647
Author Suenaga, Kazu
Thang, Ho Viet
Fang, Huihuang
Zheng, Jianwei
Fellowes, Joshua
Tsang, Shik Chi Edman
Kato, Ryuichi
Ayvali, Tugce
Reyes, Yves Ira A.
Leung, Kwan Chee
Large, Alexander
Ho, Ping-Luen
Held, Georg
Wu, Simson
Chen, Hsin-Yi Tiffany
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  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
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  surname: Wu
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  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
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  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
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  surname: Zheng
  fullname: Zheng, Jianwei
  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
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  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
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  surname: Leung
  fullname: Leung, Kwan Chee
  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
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  orcidid: 0000-0001-8676-4172
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  fullname: Large, Alexander
  organization: Diamond Light Source
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  surname: Held
  fullname: Held, Georg
  organization: Diamond Light Source
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  givenname: Ryuichi
  surname: Kato
  fullname: Kato, Ryuichi
  organization: National Institute of Advanced Industrial Science and Technology (AIST)
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  surname: Suenaga
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  organization: National Institute of Advanced Industrial Science and Technology (AIST)
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  givenname: Ho Viet
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  fullname: Thang, Ho Viet
  organization: The University of Danang, University of Science and Technology
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  orcidid: 0000-0002-9651-3200
  surname: Chen
  fullname: Chen, Hsin-Yi Tiffany
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  givenname: Shik Chi Edman
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  fullname: Tsang, Shik Chi Edman
  email: edman.tsang@chem.ox.ac.uk
  organization: The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford
BackLink https://www.ncbi.nlm.nih.gov/pubmed/36746965$$D View this record in MEDLINE/PubMed
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Snippet Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient...
Ruthenium-based materials show promising performance for ammonia decomposition, yet the underlying mechanism remains to be further explored. Here the authors...
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SubjectTerms 119/118
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639/301/299
639/4077/4079/4088/4089
639/638/77/887
Ammonia
Bimetals
Catalysts
Clusters
Decomposition
Dehydrogenation
Dispersion
Humanities and Social Sciences
Hydrogen storage
Magnesium oxide
Metals
multidisciplinary
Nanoparticles
Renewable energy
Ruthenium
Science
Science (multidisciplinary)
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Title Dispersed surface Ru ensembles on MgO(111) for catalytic ammonia decomposition
URI https://link.springer.com/article/10.1038/s41467-023-36339-w
https://www.ncbi.nlm.nih.gov/pubmed/36746965
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https://www.proquest.com/docview/2774269161
https://pubmed.ncbi.nlm.nih.gov/PMC9902439
https://doaj.org/article/c5e6c0ce7c13476baed44be11c17bf04
Volume 14
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