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• W2069926311 abstract "Turnover rates for the catalytic dehydrogenation and dehydration of formic acid (HCOOH) on NiSiO2 and Ni and CuNi powders between 390 and 490K are reported. The decomposition rate constants calculated from these data are compared with values reported previously for the temperature-programmed decomposition (TPD) of HCOOH preadsorbed on Ni and CuNi. On these, catalytic dehydrogenation and dehydration seem to proceed through the same intermediate, believed to be a formate ion. The selectivity S, defined as the ratio of dehydrogenation to dehydration turnover rates, is independent of temperature, and between 4 and 6 on Ni and alloys with a surface Cu fraction less than 0.8. The observed selectivity is not affected by secondary reactions among the products. The intermediate appears to be bound to two adjacent Ni atoms. In contrast, TPD of HCOOH preadsorbed at low coverage on CuNi single crystals seems to involve a formic anhydride species that requires four adjacent Ni atoms, and decomposes with S equal to unity and a rate constant 5 × 103 times greater than that corresponding to the catalytic decomposition. Differences between catalytic and TPD data apparently arise from the effect of surface coverage on the relative surface density of formate and formic anhydride. Formate requires small nickel ensembles and predominates on fully covered surfaces typical of the catalytic reaction. This study demonstrates the differences in rate constant and S when reactive intermediates change with surface coverage because they require different ensembles for adsorption; in other words, they are structure sensitive." @default.
• W2069926311 created "2016-06-24" @default.
• W2069926311 creator A5086150545 @default.
• W2069926311 date "1983-05-01" @default.
• W2069926311 modified "2023-10-17" @default.
• W2069926311 title "Decomposition of formic acid on copper, nickel, and copper-nickel alloys III. Catalytic decomposition on nickel and copper-nickel alloys" @default.
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• W2069926311 doi "https://doi.org/10.1016/0021-9517(83)90160-4" @default.
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