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 synthesi...

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Bibliographic Details
Published in:Chemical science (Cambridge) 2021-12, Vol.13 (1), p.5-58
Main Authors: 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
Format: Article
Language:English
Subjects:
Chemistry
Copper
Formic acid
Metal-organic frameworks
Nanoclusters
Reforming
Synthesis
System effectiveness
Zirconium
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Summary: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 controlled synthesis of novel bi- and trinuclear Cu-oxo nanoclusters supported on UiO-66-NH 2 that show notably different catalytic properties in the photocatalytic formic acid decomposition reaction is reported.
ISSN:2041-6520
2041-6539
DOI:10.1039/d1sc05495c