Structure of the catalytically active copper–ceria interfacial perimeter
By Aling Chen, Xiaojuan Yu, Yan Zhou, S. Miao, Yong Li, Sebastian Kuld, J. Sehested, J. Liu, T. Aoki, Song-Il Hong and 9 more. Nature Catalysis, 2019
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Cu/CeO2 catalysts are highly active for the low-temperature water–gas shift—a core reaction in syngas chemistry for tuning the H2/CO/CO2 proportions in feed streams—but the direct identification and quantitative description of the active sites remain challenging. Here we report that the active copper clusters consist of a bottom layer of mainly Cu+ atoms bonded on the oxygen vacancies (Ov) of ceria, in a form of Cu+–Ov–Ce3+, and a top layer of Cu0 atoms coordinated with the underlying Cu+ atoms. This atomic structure model is based on directly observing copper clusters dispersed on ceria by a combination of scanning transmission electron microscopy and electron energy loss spectroscopy, in situ probing of the interfacial copper–ceria bonding environment by infrared spectroscopy and rationalization by density functional theory calculations. These results, together with reaction kinetics, reveal that the reaction occurs at the copper–ceria interfacial perimeter via a site cooperation mechanism: the Cu+ site chemically adsorbs CO whereas the neighbouring Ov–Ce3+ site dissociatively activates H2O.Copper on ceria is an excellent catalyst for the low-temperature water–gas shift reaction. Here the active sites are directly imaged by electron microscopy and probed with in situ spectroscopy, showing that the reaction proceeds via a cooperative mechanism whereby the Cu+ chemically adsorbs CO while an adjacent Ov–Ce3+ site dissociatively activates H2O.
Subfields: Catalysis, Materials Chemistry, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/9ae3719ab9b23a0efdaebdd25550b4033a15337f
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Citations in the corpus
- Tracking the formation, fate and consequence for catalytic activity of Pt single sites on CeO2 (2020, result): “Previous results indicate that the IRband at about 2170 cm can be attributed to the CO adsorption at Ce defect sites.(43) This assignment could be confirmed also in the present study, with pure ceria showing one distinct feature at 2168 cm (Fig.”