Discovery of new destabilized hydrides for reversible hydrogen storage using first principles calculations

FUEL 106

David Sholl, sholl+@andrew.cmu.edu1, Sudhakar Alapati, asudhakar@andrew.cmu.edu2, Bing Dai, bdai@puccini.che.pitt.edu3, and J. Karl Johnson, karlj@pitt.edu3. (1) Department of Chemical Engineering, Carnegie Mellon, Pittsburgh, PA, (2) Department of Chemical Engineering, Carnegie Mellon University, 5000 Forbes Ave., Pittsburgh, PA 15213, (3) Department of Chemical and Petroleum Engineering, University of Pittsburgh, University of Pittsburgh, 1249 Benedum Hall, Pittsburgh, PA 15261
Destabilized metal hydrides provide one of the most promising routes to simultaneously achieving the goals of finding materials with high hydrogen storage capacities and materials that reversibly release and take up hydrogen under mild conditions. Although a very large number of destabilized hydrides can be conceived, the lack of thermodynamic data for many compounds of interest has limited the number of reactions whose properties can be predicted prior to experiments. We have used first-principles calculations to examine the reaction thermodynamics for a database of hundreds of potential destabilized hydrides. These calculations correctly identify the promising materials that were known from previous experiments, but more importantly, they also identify a number of other promising reactions for which no prior experimental data was available. We will discuss how our computational database can be updated as new crystal structures become available to rapidly identify new materials combination for forming destabilized hydrides. We will also describe how we have extended our calculations to consider the circumstances under which doping of stoichiometric materials can be used to tune reaction thermodynamics in these systems.