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Science 17 November 2006:
Vol. 314. no. 5802, pp. 1124 - 1126
DOI: 10.1126/science.1134230
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Reports

Reversible, Metal-Free Hydrogen Activation

Gregory C. Welch, Ronan R. San Juan, Jason D. Masuda, Douglas W. Stephan*

Although reversible covalent activation of molecular hydrogen (H2) is a common reaction at transition metal centers, it has proven elusive in compounds of the lighter elements. We report that the compound (C6H2Me3)2PH(C6F4)BH(C6F5)2 (Me, methyl), which we derived through an unusual reaction involving dimesitylphosphine substitution at a para carbon of tris(pentafluorophenyl) borane, cleanly loses H2 at temperatures above 100°C. Preliminary kinetic studies reveal this process to be first order. Remarkably, the dehydrogenated product (C6H2Me3)2P(C6F4)B(C6F5)2 is stable and reacts with 1 atmosphere of H2 at 25°C to reform the starting complex. Deuteration studies were also carried out to probe the mechanism.

Department of Chemistry and Biochemistry, University of Windsor, Windsor, Ontario N9B 3P4, Canada.

* To whom correspondence should be addressed. E-mail: stephan{at}uwindsor.ca

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