Methane oxidation activity and nanoscale characterization of Pd/CeO2 catalysts prepared by dry milling Pd acetate and ceria

被引:91
作者
Danielis, Maila [1 ,2 ]
Betancourt, Luis E. [3 ]
Orozco, Ivan [4 ]
Divins, Nuria J. [5 ,6 ]
Llorca, Jordi [5 ,6 ]
Rodriguez, Jose A. [3 ,4 ]
Senanayake, Sanjaya D. [3 ]
Colussi, Sara [1 ,2 ]
Trovarelli, Alessandro [1 ,2 ]
机构
[1] Univ Udine, Dipartimento Politecn, Via Cotonificio 108, I-33100 Udine, Italy
[2] INSTM, Via Cotonificio 108, I-33100 Udine, Italy
[3] Brookhaven Natl Lab, Div Chem, Upton, NY 11973 USA
[4] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA
[5] Univ Politecn Cataluna, EEBE, Dept Chem Engn, Inst Energy Technol, Eduard Maristany 10-14, Barcelona 08019, Spain
[6] Univ Politecn Cataluna, EEBE, Barcelona Res Ctr Multiscale Sci & Engn, Eduard Maristany 10-14, Barcelona 08019, Spain
关键词
Mechanochemistry; Methane; Palladium; Ceria; Oxidation; H BOND ACTIVATION; ENHANCED ACTIVITY; SUBSTITUTED CEO2; REDOX BEHAVIOR; CO ADSORPTION; SURFACE-AREA; PALLADIUM; COMBUSTION; METAL; TEMPERATURE;
D O I
10.1016/j.apcatb.2020.119567
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The milling of Palladium acetate and CeO2 under dry conditions results in robust, environmentally friendly catalysts with excellent methane oxidation activity. These catalysts show superior performance compared to those prepared by milling metallic Pd and outperform Pd/CeO2 catalysts prepared by traditional incipient wetness technology. Morphological investigation by HRTEM, Raman and DRIFT spectroscopic analysis, in-situ synchrotron X-ray diffraction (XRD) and X-ray absorption fine structure (XAFS) characterization techniques, coupled with ambient pressure XPS analysis, have been used to deeply characterize the samples, and allowed to identify the presence of Pd-0/Pd2+ species with different degrees of interaction with ceria (Ce3+/Ce4+). These Pd species are likely generated by the mechanical and electronic interplay taking place over the ceria surface during milling and are indicated as responsible for the enhanced catalytic activity.
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页数:13
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