Abstract

A pulse chemisorption/reaction system in combination with Fourier transform infrared spectrometer equipped with a diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) reaction cell and online mass spectrometer is described in detail. Such a system provides an approach to effectively suppress the interference of the gas-phase reactants to the vibrational signals of surface adsorbates during the operando DRIFTS measurements and, thus, allows for in situ and real-time monitor of surface species on catalyst surfaces during chemisorption/reaction processes. Employing this system, we successfully acquired DRIFTS spectra that clearly demonstrate surface species formed by propylene chemisorption and reaction on octahedral Cu2O nanocrystals; we also observed simultaneous chemisorption of CO on top, twofold, and threefold bridged sites of Pd nanoparticles supported on SiO2 upon the collision of CO prior to the saturation of strongly bound sites and the transformation of weakly bound CO(a) into strongly bound CO(a) during the dynamic chemisorption-desorption processes.

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