Understanding the Reducibility of CeO 2 Surfaces by Proton-Electron Transfer from CpCr(CO) 3 H
CeO is a popular material in heterogeneous catalysis, molecular sensors, and electronics and owes many of its special properties to the redox activity of Ce, present as both Ce and Ce . However, the reduction of CeO with H (thought to occur through proton-electron transfer (PET) giving Ce and new OH...
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| Published in: | Inorganic chemistry |
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| Main Authors: | , , , , , , |
| Format: | Journal Article |
| Language: | English |
| Published: |
United States
22.04.2024
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| ISSN: | 1520-510X |
| Online Access: | Get more information |
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| Summary: | CeO
is a popular material in heterogeneous catalysis, molecular sensors, and electronics and owes many of its special properties to the redox activity of Ce, present as both Ce
and Ce
. However, the reduction of CeO
with H
(thought to occur through proton-electron transfer (PET) giving Ce
and new OH bonds) is poorly understood due to the high reduction temperatures necessary and the ill-defined nature of the hydrogen atom sources typically used. We have previously shown that transition-metal hydrides with weak M-H bonds react with reducible metal oxides at room temperature by PET. Here, we show that CpCr(CO)
H (
) transfers protons and electrons to CeO
due to its weak Cr-H bond. We can titrate CeO
with
and measure not only the number of surface Ce
sites formed (in agreement with X-ray absorption spectroscopy) but also the lower limit of the hydrogen atom adsorption free energy (HAFE). The results match the extent of reduction achieved from H
treatment and hydrogen spillover on CeO
in a wide range of applications. |
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| ISSN: | 1520-510X |
| DOI: | 10.1021/acs.inorgchem.4c01199 |