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Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity
Ultralow stability of gold clusters prohibits the understanding of their intrinsic reactivity (that is vital for revealing the origin of gold’s catalytic properties). Using density functional theory including many-body dispersion method, we aim to ascertain effective ways in exploiting gold clusters...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group
2015
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4602230/ https://www.ncbi.nlm.nih.gov/pubmed/26459871 http://dx.doi.org/10.1038/srep15095 |
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author | Gao, Wang Ting Cui, Ting Fu Zhu, Yong Wen, Zi Zhao, Ming Chen Li, Jian Jiang, Qing |
author_facet | Gao, Wang Ting Cui, Ting Fu Zhu, Yong Wen, Zi Zhao, Ming Chen Li, Jian Jiang, Qing |
author_sort | Gao, Wang |
collection | PubMed |
description | Ultralow stability of gold clusters prohibits the understanding of their intrinsic reactivity (that is vital for revealing the origin of gold’s catalytic properties). Using density functional theory including many-body dispersion method, we aim to ascertain effective ways in exploiting gold clusters’ intrinsic reactivity on carbon nanotubes (CNTs). We find that the many body van der Waals interactions are essential for gold clusters’ reactivity on CNTs and even for O(2) activation on these supported clusters. Furthermore, curvature and dopant of CNTs are found to qualitatively change the balance between physisorption and chemisorption for gold clusters on CNTs, determining the clusters’ morphology, charge states, stability, and reactivity, which rationalize the experimental findings. Remarkably, N doped small curvature CNTs, which effectively stabilize gold clusters and retain their inherent geometric/electronic structures, can be promising candidates for exploiting gold clusters’ intrinsic reactivity. |
format | Online Article Text |
id | pubmed-4602230 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2015 |
publisher | Nature Publishing Group |
record_format | MEDLINE/PubMed |
spelling | pubmed-46022302015-10-23 Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity Gao, Wang Ting Cui, Ting Fu Zhu, Yong Wen, Zi Zhao, Ming Chen Li, Jian Jiang, Qing Sci Rep Article Ultralow stability of gold clusters prohibits the understanding of their intrinsic reactivity (that is vital for revealing the origin of gold’s catalytic properties). Using density functional theory including many-body dispersion method, we aim to ascertain effective ways in exploiting gold clusters’ intrinsic reactivity on carbon nanotubes (CNTs). We find that the many body van der Waals interactions are essential for gold clusters’ reactivity on CNTs and even for O(2) activation on these supported clusters. Furthermore, curvature and dopant of CNTs are found to qualitatively change the balance between physisorption and chemisorption for gold clusters on CNTs, determining the clusters’ morphology, charge states, stability, and reactivity, which rationalize the experimental findings. Remarkably, N doped small curvature CNTs, which effectively stabilize gold clusters and retain their inherent geometric/electronic structures, can be promising candidates for exploiting gold clusters’ intrinsic reactivity. Nature Publishing Group 2015-10-13 /pmc/articles/PMC4602230/ /pubmed/26459871 http://dx.doi.org/10.1038/srep15095 Text en Copyright © 2015, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
spellingShingle | Article Gao, Wang Ting Cui, Ting Fu Zhu, Yong Wen, Zi Zhao, Ming Chen Li, Jian Jiang, Qing Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity |
title | Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity |
title_full | Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity |
title_fullStr | Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity |
title_full_unstemmed | Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity |
title_short | Design Principles of Inert Substrates for Exploiting Gold Clusters’ Intrinsic Catalytic Reactivity |
title_sort | design principles of inert substrates for exploiting gold clusters’ intrinsic catalytic reactivity |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4602230/ https://www.ncbi.nlm.nih.gov/pubmed/26459871 http://dx.doi.org/10.1038/srep15095 |
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