Bound to Give an Explanation

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Science  25 May 2001:
Vol. 292, Issue 5521, pp. 1453
DOI: 10.1126/science.292.5521.1453a

Often, reactions in solution are better characterized than those on surfaces, in part because solution species tend to be homogenous and can be probed in bulk with analytical and spectroscopic methods. Gallagher and Meyer provide an example in which binding of a reactant to a surface leads not only to mechanistic insights but also to greater control over the reaction, in this case a partial oxidation by a RuIV-oxo complex. In solution, two-electron (2e) oxidation forms RuII, but this species reacts rapidly with RuIV to produce the RuIII that is observed. However, when tethered to a TiO2 surface grown on glass, the disproportionation reaction is slowed, and the RuII species can be detected by ultraviolet-visible spectroscopy. Surface binding also helps limit the reaction with organic species to a single 2e oxidation. Thus, whereas cyclohexene in solution is oxidized to the ketone, the surface-bound complex yields primarily the alcohol. — PDS

J. Am. Chem. Soc., in press.

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