The
redox properties of supported Pd catalysts can directly affect
their methane combustion activity. Here, the effect of the support
on methane combustion was elucidated using Pd nanoparticles supported
on various metal oxides (θ-Al2O3, γ-Al2O3, ZrO2, CeO2, MgO, La2O3, TiO2, SnO2, and Nb2O5). To eliminate the effect of Pd particle size
and morphology, uniform Pd particles were synthesized in the liquid
phase. Interestingly, the methane combustion activity formed a volcano
plot when plotted against the oxide formation enthalpy (Δf
H
M‑O°) of the support.
Combining X-ray photoelectron spectroscopy and scanning transmission
electron microscopy–electron energy loss spectroscopy, the
structure of the Pd nanoparticles on the support in an oxidizing atmosphere
was identified. Pd particles on θ-Al2O3, γ-Al2O3, ZrO2, and CeO2 with moderate Δf
H
M‑O° adopted a metal-core–oxide-shell structure and showed
the highest activities for methane combustion. In contrast, completely
oxidized Pd particles were present on MgO and La2O3, which have lower Δf
H
M‑O° and were not very active. Pd metal particles
on TiO2, SnO2, and Nb2O5 with higher Δf
H
M‑O° were not effective catalysts for methane combustion.
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