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• W2024886218 startingPage "6573" @default.
• W2024886218 abstract "Gas-phase hydrogen radicals cause desulfurization of the sulfided Ni(100) surface even for temperatures as low as 120 K, resulting in H2S formation. In contrast, no thermal desulfurization is observed in the presence of coadsorbed hydrogen. During hydrogen radical exposure, sulfur is abstracted from the Ni(100) surface by a sequential Eley−Rideal mechanism. After hydrogen radical exposure, two additional H2S formation pathways involving coadsorbed hydrogen are observed during subsequent heating. In the first pathway, H2S formation is observed at 150 K, involving a partially hydrogenated intermediate formed during gas-phase atomic hydrogen exposure. The second pathway involves addition of desorbing subsurface hydrogen to adsorbed sulfur, leading to H2S formation at 190 K. Both the temperature and coverage dependence of the 150 K pathway support a sequential hydrogen addition mechanism with a sulfhydryl intermediate during temperature-programmed desorption (TPD) studies. Previous H2S decomposition studies on this surface show that the sulfhydryl intermediate is not stable above ∼190 K because of thermal dehydrogenation. The temperature dependence of H2S formation and sulfur removal during exposure to the gas-phase hydrogen radical is also consistent with a sulfhydryl intermediate. Above 200 K, no desulfurization is observed during gas-phase hydrogen radical exposure. This thermal dehydrogenation of H2S also depends on the coverage of coadsorbed sulfur. Increasing sulfur coverages inhibits dehydrogenation of both H2S and SH. With higher sulfur coverages, H2S desorption is favored and substantial sulfur is removed during temperature-programmed reaction spectroscopy (TPRS) experiments after low-temperature hydrogen radical exposure. Taken together, the temperature- and coverage-dependent behavior indicates that sulfhydryl is an intermediate for sulfur abstraction. Through control of gas-phase hydrogen radical exposure, vacancies in sulfided nickel layers were generated. Hydrogen chemisorption studies were used to probe these sulfur vacancies. The new, low-temperature hydrogen desorption peak at 230 K corresponds to hydrogen modified by coadsorbed sulfur." @default.
• W2024886218 created "2016-06-24" @default.
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• W2024886218 date "1999-07-20" @default.
• W2024886218 modified "2023-10-17" @default.
• W2024886218 title "Desulfurization of the Ni(100) Surface Using Gas-Phase Hydrogen Radicals" @default.
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• W2024886218 doi "https://doi.org/10.1021/jp990937q" @default.
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