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Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations

Precisely tuning the nuclearity of supported metal nanoclusters is pivotal for designing more superior catalytic systems, but it remains practically challenging. By utilising the chemical and molecular specificity of UiO-66-NH(2) (a Zr-based metal–organic framework), we report the controlled synthes...

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Autores principales: Xue, Qi, Ng, Bryan Kit Yue, Man, Ho Wing, Wu, Tai-Sing, Soo, Yun-Liang, Li, Molly Mengjung, Kawaguchi, Shogo, Wong, Kwok Yin, Tsang, Shik Chi Edman, Huang, Bolong, Lo, Tsz Woon Benedict
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8694280/
https://www.ncbi.nlm.nih.gov/pubmed/35059150
http://dx.doi.org/10.1039/d1sc05495c
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author Xue, Qi
Ng, Bryan Kit Yue
Man, Ho Wing
Wu, Tai-Sing
Soo, Yun-Liang
Li, Molly Mengjung
Kawaguchi, Shogo
Wong, Kwok Yin
Tsang, Shik Chi Edman
Huang, Bolong
Lo, Tsz Woon Benedict
author_facet Xue, Qi
Ng, Bryan Kit Yue
Man, Ho Wing
Wu, Tai-Sing
Soo, Yun-Liang
Li, Molly Mengjung
Kawaguchi, Shogo
Wong, Kwok Yin
Tsang, Shik Chi Edman
Huang, Bolong
Lo, Tsz Woon Benedict
author_sort Xue, Qi
collection PubMed
description Precisely tuning the nuclearity of supported metal nanoclusters is pivotal for designing more superior catalytic systems, but it remains practically challenging. By utilising the chemical and molecular specificity of UiO-66-NH(2) (a Zr-based metal–organic framework), we report the controlled synthesis of supported bi- and trinuclear Cu-oxo nanoclusters on the Zr(6)O(4) nodal centres of UiO-66-NH(2). We revealed the interplay between the surface structures of the active sites, adsorption configurations, catalytic reactivities and associated reaction energetics of structurally related Cu-based ‘single atoms’ and bi- and trinuclear species over our model photocatalytic formic acid reforming reaction. This work will offer practical insight that fills the critical knowledge gap in the design and engineering of new-generation atomic and nanocluster catalysts. The precise control of the structure and surface sensitivities is important as it can effectively lead to more reactive and selective catalytic systems. The supported bi- and trinuclear Cu-oxo nanoclusters exhibit notably different catalytic properties compared with the mononuclear ‘Cu(1)’ analogue, which provides critical insight for the engineering of more superior catalytic systems.
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spelling pubmed-86942802022-01-19 Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations Xue, Qi Ng, Bryan Kit Yue Man, Ho Wing Wu, Tai-Sing Soo, Yun-Liang Li, Molly Mengjung Kawaguchi, Shogo Wong, Kwok Yin Tsang, Shik Chi Edman Huang, Bolong Lo, Tsz Woon Benedict Chem Sci Chemistry Precisely tuning the nuclearity of supported metal nanoclusters is pivotal for designing more superior catalytic systems, but it remains practically challenging. By utilising the chemical and molecular specificity of UiO-66-NH(2) (a Zr-based metal–organic framework), we report the controlled synthesis of supported bi- and trinuclear Cu-oxo nanoclusters on the Zr(6)O(4) nodal centres of UiO-66-NH(2). We revealed the interplay between the surface structures of the active sites, adsorption configurations, catalytic reactivities and associated reaction energetics of structurally related Cu-based ‘single atoms’ and bi- and trinuclear species over our model photocatalytic formic acid reforming reaction. This work will offer practical insight that fills the critical knowledge gap in the design and engineering of new-generation atomic and nanocluster catalysts. The precise control of the structure and surface sensitivities is important as it can effectively lead to more reactive and selective catalytic systems. The supported bi- and trinuclear Cu-oxo nanoclusters exhibit notably different catalytic properties compared with the mononuclear ‘Cu(1)’ analogue, which provides critical insight for the engineering of more superior catalytic systems. The Royal Society of Chemistry 2021-11-29 /pmc/articles/PMC8694280/ /pubmed/35059150 http://dx.doi.org/10.1039/d1sc05495c Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/
spellingShingle Chemistry
Xue, Qi
Ng, Bryan Kit Yue
Man, Ho Wing
Wu, Tai-Sing
Soo, Yun-Liang
Li, Molly Mengjung
Kawaguchi, Shogo
Wong, Kwok Yin
Tsang, Shik Chi Edman
Huang, Bolong
Lo, Tsz Woon Benedict
Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
title Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
title_full Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
title_fullStr Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
title_full_unstemmed Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
title_short Controlled synthesis of Bi- and tri-nuclear Cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
title_sort controlled synthesis of bi- and tri-nuclear cu-oxo nanoclusters on metal–organic frameworks and the structure–reactivity correlations
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8694280/
https://www.ncbi.nlm.nih.gov/pubmed/35059150
http://dx.doi.org/10.1039/d1sc05495c
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