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Title: in situ high pressure XRD study on hydrogen uptake behavior of Pd-Carbon systems

Conference ·

Efficient storage of hydrogen for use in fuel cell-powered vehicles is a challenge that is being addressed in different ways, including adsorptive, compressive, and liquid storage approaches. Some of the work in this respect at Oak Ridge National Laboratory is directed towards adsorptive storage in nanoporous carbon fibers in which palladium is incorporated prior to spinning and carbonization/activation of the fibers. Nanoparticles of Pd, when dispersed in activated carbon fibers (ACF), enhance the hydrogen storage capacity of ACF. Adsorption capacity of Pd-ACF increases with increasing temperature below 0.4 bar, and the trend reverses when the pressure increases. To understand the cause for such behavior, hydrogen uptake properties of Pd with different degrees of Pd-carbon contact (Pd deposited on carbon surface and Pd embedded in carbon matrix) are compared with Pd-sponge using in situ XRD under various hydrogen partial pressures (<10 bar). Rietveld refinement and profile analysis of diffraction patterns does not show any significant changes in carbon structure even under 10 bar H2. Pd forms PdH0.67 under 10 bar H2, which transforms to PdH0.02 as the hydrogen partial pressure is decreased. However, the equilibrium pressure of transition (corresponding to a 1:1 ratio of and phases) increases with increasing the extent of Pd-carbon contact. This pressure is higher for Pd embedded in carbon than for Pd deposited on carbon surface. Both these Pd-carbon materials have higher H2 desorption pressure than pure Pd, indicating that carbon pumps out hydrogen from PdHx and the pumping power depends on the extent of Pd-carbon contact. These results support the spillover mechanism (dissociative adsorption of H2 followed by surface diffusion of atomic H).

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE Office of Science (SC)
DOE Contract Number:
AC05-00OR22725
OSTI ID:
1364244
Resource Relation:
Journal Volume: 1042; Conference: MRS Fall 2007 meeting, Boston, MA, USA, 20071127, 20071129
Country of Publication:
United States
Language:
English