Outstanding Methane Oxidation Performance of Palladium-Embedded Ceria Catalysts Prepared by a One-Step Dry Ball-Milling Method

被引:151
作者
Danielis, Maila [1 ]
Colussi, Sara [1 ]
de Leitenburg, Carla [1 ]
Soler, Lluis [2 ,3 ]
Llorca, Jordi [2 ,3 ]
Trovarelli, Alessandro [1 ]
机构
[1] Univ Udine, Polytech Dept, Via Cotonificio 108, I-33100 Udine, Italy
[2] Univ Politecn Cataluna, Inst Energy Technol, Dept Chem Engn, EEBE Eduard Maristany 10-14, Barcelona 08019, Spain
[3] Univ Politecn Cataluna, Barcelona Res Ctr Multiscale Sci & Engn, EEBE Eduard Maristany 10-14, Barcelona 08019, Spain
关键词
ceria; combustion; mechanochemistry; methane; palladium; CO OXIDATION; CH4; OXIDATION; COMBUSTION; NANOPARTICLES; SITES; STATE; IONS;
D O I
10.1002/anie.201805929
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
By carefully mixing Pd metal nanoparticles with CeO2 polycrystalline powder under dry conditions, an unpredicted arrangement of the Pd-O-Ce interface is obtained in which an amorphous shell containing palladium species dissolved in ceria is covering a core of CeO2 particles. The robust contact that is generated at the nanoscale, along with mechanical forces generated during mixing, promotes the redox exchange between Pd and CeO2 and creates highly reactive and stable sites constituted by PdOx embedded into CeO2 surface layers. This specific arrangement outperforms conventional Pd/CeO2 reference catalysts in methane oxidation by lowering light-off temperature by more than 50 degrees C and boosting the reaction rate. The origin of the outstanding activity is traced to the structural properties of the interface, modified at the nanoscale by mechanochemical interaction.
引用
收藏
页码:10212 / 10216
页数:5
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