ABSTRACT PdO serves as the primary active phase in Pd‐based catalysts for CH 4 combustion, and the low‐temperature elimination is not achieved due to the difficult activation of surface lattice oxygen. Herein, we design Ni‐modified PdO catalytic structure with Pd‐O‐Ni sites and optimize the modified amount of Ni. This catalytic structure promotes the activation of surface lattice oxygen via Pd‐O‐Ni sites. This catalytic site accelerates the conversion of monodentate carbonate to achieve the modulation of reaction pathway compared to Pd/CeO 2 . DFT calculations indicate that Ni donates abundant electrons to PdO, thereby weakening the Pd‐O bond and forming active Pd‐O‐Ni sites. This reactive site enables the activation energy for CH 4 dissociation on PdNi/CeO 2 (0.39 eV) to be lower than that on Pd/CeO 2 (0.61 eV). As a result, PdNi/CeO 2 exhibits lower T 90 value (375°C vs. 425°C) and apparent activation energy (91.7 kJ/mol vs. 120.0 kJ/mol) than Pd/CeO 2 for CH 4 combustion.
Wang et al. (Fri,) studied this question.