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• W4289261342 abstract "Here, we report the photoelectron-induced excitation (PEIE) spectroscopy and its close correlation with fundamental studies of catalysis. In the PEIE spectroscopy, a spectrum is formed through scattering free molecules of the on-site gas phase proximal to a catalyst surface by an electron source generated from the catalyst surface. The electron source is these photoelectrons with a specific kinetic energy (KE) released from the catalyst surface such as Pt 4f7/2 from a Pt catalyst or C 1s photoelectrons from graphite. Pt, Au, Ag, and graphite were used as catalysts in this work; CO, O2, N2, or their mixtures were used as a pure gas or gaseous mixtures around a catalyst surface. A constituting peak in a PEIE spectrum is contributed by photoelectrons that lose a certain amount of KE (ΔE) after scattering free molecules of the on-site gas phase proximal to the catalyst surface in the space of zero to submillimeters. By measuring the kinetic energies KEf of these photoelectrons after scattering with gaseous molecules, ΔE are identified. As ΔE is the energy used for exciting free molecules from their ground state to a specific excitation state, the identification of ΔE of these peaks of a PEIE spectrum allows us to build the energy diagram of molecular orbitals of the on-site gas phase proximal to the catalyst surface. With the composed energy diagram of a molecule, the molecular identity of the gas can be obtained by comparing it to references. The PEIE spectroscopy allows for observing both occupied and unoccupied molecular orbitals of molecules in a gas phase. Intensity of the PEIE spectrum is proportional to intensity of electron source in terms of photoelectrons and density of molecules in gas phase. As the intensity of a PEIE spectrum of a gas is proportional to molecular density of gas in terms of this partial pressure of the on-site gas proximal to the catalyst surface, PEIE spectroscopy can be used to measure the gas pressure and analyze the composition of an on-site gas mixture proximal to a catalyst surface. It is expected that PEIE spectroscopy is particularly valuable for high-temperature catalysis because the identity of constituting gases and composition of an on-site high-temperature gas phase proximal to the high-temperature catalyst surface during catalysis can be different from those of an off-site gas phase characterized at a low temperature or room temperature. In addition, it is expected that it can identify radical species formed in the on-site gas phase around the catalyst surface at high temperature. Because the parent peak(s) of a PEIE extended spectrum represent the surface chemistry of the catalyst and the PEIE difference spectrum provides information on molecular identity and partial pressure of constituting gases of the on-site gas proximal to a working catalyst surface, the integration of PEIE spectroscopy with ambient pressure X-ray photoelectron spectroscopy offers a significant function of both characterizing a catalyst surface and simultaneously measuring the on-site catalytic performance of the catalyst in terms of on-site turn-over rate (TOR) during catalysis for gaining a fundamental understanding of a catalytic reaction with a real-time manner of spatial proximity and temporal simultaneity." @default.
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• W4289261342 date "2022-08-01" @default.
• W4289261342 modified "2023-10-11" @default.
• W4289261342 title "Report on Photoelectron-Induced Excitation Spectroscopy and Its Close Correlation with Fundamental Studies of Catalysis" @default.
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• W4289261342 doi "https://doi.org/10.1021/acs.jpcc.2c00209" @default.
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