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• W2023735978 abstract "Exposure of Pd-based hydrogen purification membranes to H2S, a common contaminant in coal gasification streams, can cause membrane performance to deteriorate, either by deactivating surface sites required for dissociative H2 adsorption or by forming a low-permeability sulfide scale. In this work, the composition, structure, and catalytic activity of Pd4S, a surface scale commonly observed in Pd−membrane separation of hydrogen from sulfur-containing gas streams, were examined using a combination of experimental characterization and density functional theory (DFT) calculations. A Pd4S sample was prepared by exposing a 100 μm Pd foil to H2S at 908 K. Both X-ray photoemission depth profiling and low energy ion scattering spectroscopic (LEISS) analysis reveal slight sulfur-enrichment of the top surface of the sample. This view is consistent with the predictions of DFT atomistic thermodynamic calculations, which identified S-terminated Pd4S surfaces as energetically favored over corresponding Pd-terminated surfaces. Activation barriers for H2 dissociation on the Pd4S surfaces were calculated. Although barriers are higher than on Pd(111), transition state theory analysis identified reaction pathways on the S-terminated surfaces for which hydrogen dissociation rates are high enough to sustain the separation process at conditions relevant to gasification applications." @default.
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• W2023735978 date "2009-10-05" @default.
• W2023735978 modified "2023-09-26" @default.
• W2023735978 title "Hydrogen Dissociation on Pd₄S Surfaces" @default.
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• W2023735978 doi "https://doi.org/10.1021/jp906694k" @default.
• W2023735978 hasPublicationYear "2009" @default.
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