DUAL SITE CATALYSTS FOR HYDRIDE MANIPULATION

Abstract

This comment describes our efforts to develop dual site catalysts for hydride manipulation. We began by analyzing the mechanism of alcohol oxidation with the ruthenium-based Shvo catalyst, which utilizes a proton transfer to template a hydride transfer from carbon to ruthenium in a single transition state. In our project we are working to extend this concept of reactivity from the use of proton transfer as a templating interaction for hydride transfer to the use of a Lewis acid to coordinate and direct a substrate to a metal. Along these lines, we have found that ammonia borane, a popular and high-weight-content hydrogen storage material, has been one of our best model substrates with which to study hydride transfer mechanisms. Our ongoing studies have thus far given new insight into the reactivity of the Shvo system, particularly regarding dehydrogenation of ammonia borane, and have enabled us to design a new, prolific, air- and water-tolerant, and reusable catalyst for ammonia borane dehydrogenation.

Keywords:

• ammonia borane
• bifunctional catalyst
• hydride
• hydrogen storage
• ruthenium
• Shvo catalyst

ACKNOWLEDGMENT

We thank the University of Southern California, the ACS Petroleum Research fund (47987-G1), the Hydrocarbon Research Foundation, and the National Science Foundation (CHE-1054910). We appreciate grants from the NSF (DBI-0821671, CHE-0840366) and NIH (S10 RR25432) to support NMR spectrometers.

Notes

^a Adapted from ref. 15.

^b Adapted from ref. 16.