1. Reaction gas-induced partial exsolution of Pd from PdCeMnO for methane combustion.
- Author
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Zhao, Han, Tan, Yuanlong, Li, Lin, Su, Yang, Wang, Aiqin, Liu, Xiao Yan, and Zhang, Tao
- Subjects
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COMBUSTION , *ALUMINUM oxide , *COMBUSTION kinetics , *PARTIAL oxidation , *CERIUM oxides , *METHANE - Abstract
• Pd is doped into the CeMnO bulk lattice by an optimized co-precipitation (CP). • CP outperforms impregnation for CH 4 combustion and CH 4 -related three-way reactions. • Pd in PdCeMnO-CP is partially exsoluted, with lowered valence, after CH 4 combustion. • Surface oxygen vacancy is enriched after CH 4 combustion over PdCeMnO-CP. Besides the Pd/Al 2 O 3 , the Pd-CeO 2 catalysts are the indispensable and promising candidates for methane combustion. The Pd-CeO 2 composites with intimate interaction realized by elaborate methods are regarded as the most active formulations. However, more facile and cost-efficient methods are needed for industrial application. Herein, the Pd was incorporated into the lattice of the Mn-doped CeO 2 by an optimized co-precipitation method to synthesize the PdCeMnO-CP catalyst. The PdCeMnO-CP showed much higher catalytic activity with the T 10 decreased by 70 °C than that of the Pd/CeMnO-Imp prepared with impregnation. The partial exsolution of the initially doped Pd species and the lowered valence of Pd (from Pd4+ to Pdδ+, δ: 2 ∼ 4) during the reaction were confirmed by the low-temperature CO-DRIFTs, CO-pulse chemisorption, XRD and XPS, which were responsible for the activity enhancement. The undercoordinated Ce4+ species were generated during the reaction, thus improving the mobility of the lattice oxygen which is vital for the methane combustion following the MvK mechanism. The PdCeMnO-CP also showed higher activity for the complex methane-containing three-way catalytic reactions than the Pd/CeMnO-Imp, demonstrating its potential for industrial application. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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