The CO oxidation reaction on the Pd(111) model catalyst at various temperatures (200–400 °C) under hundreds mTorr pressure conditions has been monitored by in situ ambient pressure X-ray photoelectron spectroscopy and mass spectroscopy. In situ observation of the reaction revealed that the Pd(111) surface is covered by CO molecules at a lower temperature (200 °C), while at higher temperatures (300–400 °C) several oxide phases are formed on the surface. We found that the reactivity is enhanced in the presence of a surface oxide and significantly suppressed by formation of a cluster oxide and the PdO bulk oxide. CO titration experiments suggest that less coordinated oxygen atoms are more reactive for CO oxidation.

We have developed a soft x-ray time-resolved photoemission spectroscopy system using synchrotron radiation (SR) at SPring-8 BL07LSU and an ultrashort pulse laser system. Two-dimensional angle-resolved measurements were performed with a time-of-flight-type analyzer. The photoemission spectroscopy system is synchronized to light pulses of SR and laser using a time control unit. The performance of the instrument is demonstrated by mapping the band structure of a Si(111) crystal over the surface Brillouin zones and observing relaxation of the surface photo-voltage effect using the pump (laser) and probe (SR) method.

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The CO oxidation reaction on Ir(111) is observed by the near-edge x-ray absorption fine structure (NEXAFS) spectroscopy in the soft x-ray region. A continuous data acquisition at 33 ms real-time resolution is realized for a single event of the reaction without the repetition, by adopting the wavelength-dispersive NEXAFS technique. The time evolution of the coverages for atomic O and molecular CO is quantitatively estimated during the reaction. The obtained activation energy is significantly larger than that on Pt(111).

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