Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 117, Issue 8, Pages 4158-4167Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp312532u
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Funding
- JSPS fellowship at Kyushu University
- EU Transnational Access Program at CenTACat group
- EPSRC under the CASTech programme
- EPSRC [EP/G012156/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/G012156/1] Funding Source: researchfish
- Grants-in-Aid for Scientific Research [11F01343] Funding Source: KAKEN
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Time-resolved DRIFTS, MS, and resistance measurements were used to study the interaction of undoped and Pd-doped SnO2 with H-2 in air and argon at 300 degrees C. Using first-order kinetics, we compare the time constants for the resistance drop and its partial recovery with those of the surface hydroxyl evolution and water formation in the gas phase upon exposure to hydrogen. In the case of the undoped oxide, resistance and bridging hydroxyls (BOHs) evolve similarly, manifesting a fast main drop followed by recovery at a similar rate. The rate of water formation for this material was found to be much slower than that of the main drop in both the resistance and BOHs. In contrast, the resistance change for SnO2-Pd appeared to be similar to that of water formation, and no correlation was found between the evolution of resistance and surface OHs. Isotopic exchange on both materials revealed that water formation occurs via fast and slow hydrogen transfer to surface oxygen species. While the former originates from just-adsorbed hydrogen, the latter appears to proceed from the preadsorbed OHs. Both surfaces exhibit close interaction between chemisorbed oxygen and existing bridging OH groups, indicating that the latter is an intermediate in the hydrogen oxidation and generation of donor states on the surface.
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