期刊
SCIENCE
卷 319, 期 5862, 页码 438-442出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1148643
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The reactivity pattern of small (similar to 10 to 20 atoms) anionic aluminum clusters with oxygen has posed a long- standing puzzle. Those clusters with an odd number of atoms tend to react much more slowly than their even- numbered counterparts. We used Fourier transform ion cyclotron resonance mass spectrometry to show that spin conservation straightforwardly accounts for this trend. The reaction rate of odd- numbered clusters increased appreciably when singlet oxygen was used in place of ground- state ( triplet) oxygen. Conversely, monohydride clusters AlnH-, in which addition of the hydrogen atom shifts the spin state by converting formerly open- shell structures to closed- shell ones ( and vice versa), exhibited an opposing trend: The odd- n hydride clusters reacted more rapidly with triplet oxygen. These findings are supported by theoretical simulations and highlight the general importance of spin selection rules in mediating cluster reactivity.
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