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Structure-Activity Map of Ceria Nanoparticles, Nanocubes and Mesoporous Architectures

Sayle, Thi X. T., Caddeo, Francesco, Zhang, Xueqiang, Sakthivel, Tamilselvan, Das, Soumen, Seal, Sudipta, Ptasinska, Sylwia, Sayle, Dean C. (2016) Structure-Activity Map of Ceria Nanoparticles, Nanocubes and Mesoporous Architectures. Chemistry of Materials, 28 (20). pp. 7287-7295. ISSN 0897-4756. (doi:10.1021/acs.chemmater.6b02536) (KAR id:56848)

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Structure-activity mapping is central to the exploitation and optimisation of nanomaterial catalysts in a variety of technologically important heterogeneous reactions, such as automotive catalysis and water gas shift reactions. Here, we present a catalytic activity map for nanoceria, calculated as a function of shape, size, architecture and defect content, using atom-level models.

The decrease in catalytic activity during an oxidation reaction - emanating from the increase in energy required to extract oxygen - suggests that there exists a ‘window of catalytic operation’, where the activity of the catalyst can be controlled by operating at different points within this window. We show experimentally, how the activity can be modified by engineering the oxygen vacancy concentration and hence the oxygen content of the catalyst to facility tunable activity.

To generate the atom-level models of ceria nanostructures, we use non-equilibrium Molecular Dynamics to simulate the self-assembly of mesoporous ceria from amorphous nano-building blocks, followed by a (simulated) crystallisation step; the latter evolves the crystal structure and microstructural features such as grain-boundaries and dislocations. Our simulated crystallisations emanate wholly from a multitude of ‘random’ atom collisions, which result in the spontaneous evolution of a crystalline seed that nucleates crystallisation of the whole system. The atomistic models generated by ‘simulating synthesis’ are shown to be in quantitative structural agreement with experiment.

Item Type: Article
DOI/Identification number: 10.1021/acs.chemmater.6b02536
Uncontrolled keywords: Functional Materials Group
Subjects: Q Science > QD Chemistry > QD478 Solid State Chemistry
Divisions: Divisions > Division of Natural Sciences > School of Physical Sciences
Depositing User: Dean Sayle
Date Deposited: 16 Aug 2016 11:32 UTC
Last Modified: 16 Feb 2021 13:36 UTC
Resource URI: (The current URI for this page, for reference purposes)
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