期刊
ACS CATALYSIS
卷 5, 期 4, 页码 2481-2489出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs502036d
关键词
homogeneous catalysis; XAFS; in situ; methane; modulation excitation
资金
- Swedish Research Council [621-2011-5009, 349-2011-6491, 349-2013-567]
- Competence Centre for Catalysis
- Swedish Energy Agency
- AB Volvo
- ECAPS AB
- Haldor Topsoe A/S
- Scania CV AB
- Volvo Car Corporation AB
- Wartsila Finland Oy
Time-resolved in situ, energy-dispersive X-ray absorption spectroscopy and mass spectrometry are used to correlate changes in the chemical state of alumina- and ceria-supported palladium nanoparticles with changes in activity and selectivity for methane oxidation. Specifically, modulation excitation spectroscopy experiments are carried out by periodically cycling between net-reducing and net-oxidizing reaction conditions. The XANES and EXAFS data show that the palladium nanoparticles are readily bulk-oxidized when exposed to oxygen, forming a PdO-like phase, and reduced back to a reduced (metal) phase when oxygen is removed from the feed. The difference between the two support materials is most noticeable at the switches between net-oxidizing and net-reducing reaction conditions. Here, a brief reduction in conversion is observed for the alumina-supported catalyst, but for the ceria-supported catalyst, this reduction in conversion is minor or not observed at all. This difference is attributed to differences in the oxidation kinetics and the oxygen storage capability of ceria.
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