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THE INTERACTION OF CARBON DIOXIDE WITH SINGLE CRYSTAL CaO(100) SURFACES

We have carried out synchrotron-based photoemission spectroscopy (O 1s, C 1s, Ca 2p, Ca 3p/O 2s/VB) and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy (C K-edge) study of the interaction of CO2 with UHV-cleaved synthetic single crystal CaO(100) surfaces. Our data are compared with data collected from a high quality natural sample of (calcite). The CaO (100) surface readily undergoes hydroxylation with the ambient pH2O associated with most UHV systems. Carbon coverages were observed to be lower for the most hydroxylated sample. Comparison of our C K-edge data for CO2/CaO(100) and calcite indicates that there is formation of a surface carbonate species at CO2 pressures above 10-6 Torr. The reaction of CaO(100) with CO2 occurs at far lower CO2 pressures than for MgO(100), which is consistent with equilibrium thermodynamic predictions.