Abstract
Inelastic neutron scattering spectra have been collected over a wide range of momentum transfer from H2 adsorbed in several high-porosity carbon substrates. We show theoretical spectra which consider the relationship between rotational and translational transitions in the highly anisotropic adsorption environment, proving that different rotational excitations contain different amount of recoil broadening and motivating a new analysis method which considers both types of transitions at once. Spectra for most of the samples, including two activated carbons, are very similar to one another, supporting models of nanoporous carbons which are quite similar on the sub-nanometer scale. The exception is the low-energy side of the rotational peak, indicating important differences in the initial distribution of motion. We also find more subtle differences in the spectra which may be linked to differences in sample heterogeneity and surface rugosity. One sample does have a very different spectrum, which is not explained by standard models of this system. We also observe a significantly reduced effective mass in the spectrum of recoil transitions and evidence of coupling of rotational and translational motion resulting from periodic variations in orientation of the rotational states.
Original language | English |
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Pages (from-to) | 46-58 |
Number of pages | 13 |
Journal | Carbon |
Volume | 58 |
DOIs | |
State | Published - Jul 2013 |
Funding
We would like to thank Enrique Robles for capable experimental assistance. This research was supported by the Department of Energy Office of Basic Energy Science (DOE-BES) under contract DE-FG02-07ER46411. Research at Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. H.T. was supported by the National Science Foundation (NSF) under contract number DMR-0705974 and DGE-1069091. R.J.O. was also supported in part by the DOE Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Awards under the EERE Fuel Cell Technologies Program, administered by the Oak Ridge Institute for Science and Education (ORISE) for the DOE. ORISE is managed by Oak Ridge Associated Universities (ORAU) under DOE contract number DEAC05-06OR23100. All opinions expressed in this paper are the authors’ and do not necessarily reflect the policies and views of DOE, ORAU, or ORISE.
Funders | Funder number |
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Department of Energy Office of Basic Energy Science | DE-FG02-07ER46411 |
Office of Basic Energy Sciences | |
Scientific User Facilities Division | |
National Science Foundation | DGE-1069091, DMR-0705974 |
U.S. Department of Energy | |
Office of Energy Efficiency and Renewable Energy | |
Fuel Cell Technologies Program | |
Oak Ridge Associated Universities | DEAC05-06OR23100 |
Oak Ridge National Laboratory | |
Oak Ridge Institute for Science and Education |