The kinetics of reactions of nickel clusters with hydrogen and deuterium |
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Authors: | W F Hoffman III E K Parks G C Nieman L G Pobo S J Riley |
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Institution: | 1. Oak Ridge National Laboratory, Chemical Physics Section, Health and Safety Research Division, Tennessee, USA
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Abstract: | The kinetics of reactions of nickel clusters with hydrogen and deuterium are studied in a laser-vaporization cluster source coupled to a continuous-flow reactor. The abslute rate constants for the addition of the first H2 (D2) molecule to nickel clusters Ni n (n=7→36 for H2 andn=7→60 for D2) have been measured. Rate constants are found to be only weakly dependent onn forn≧14, showing a gradual increase with size that scales approximately withn (2/3), i.e., the cluster geometrical cross section. Reaction probabilities for clusters in this size range are approximately 0.6 for H2 and 0.3 for D2. Belown=14, there is a stronger dependence of reactivity on size, with Ni9 being far less reactive than any other cluster studied. These results are compared to bulk nickel studies, and a discussion of possible correlation of reactivity to cluster structure is presented. |
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