462282 Nitrogen Interaction with Various 1D and 3D Nanostructured Carbon Architectures Probed VIA in-SITU Vibrational Spectroscopy

Tuesday, November 15, 2016: 5:20 PM
Cyril Magnin II (Parc 55 San Francisco)
Paramita Ray, Intel, Hillsboro, OR, Angela D. Lueking, Energy and Geo-Environmental Engineering, Pennsylvania State University, State College, PA, John V. Badding, Chemistry, The Pennsylvania State University, University Park, PA, Enshi Xu, The Pennsylvania State University, University Park, PA and Vincent H. Crespi, Physics, The Pennsylvania State University, University Park, PA

The study utilizes in-situ vibrational spectroscopy to probe nitrogen adsorption to porous carbon materials. Combined theoretical and experimental studies demonstrate how the nitrogen vibrational spectra becomes perturbed by a carbon surface as well as nearest neighbor gas molecules. The perturbation is sensitive to gas-surface binding energy, pore structure, and surface chemistry. As the pore dimension of a Polymer of Intrinsic Microporosity (PIM-1) is reduced via photochemical irradiation, the position and intensity of the perturbation tracks the pore dimension. Chemical alteration of the PIM-1 surface, along with control studies with nonporous analogs, elucidates the role of surface chemistry, demonstrating π-π stacking interactions between the C-N group and the N-N triple bond. The nitrogen spectra is similarly perturbed in non-functionalized activated carbon and single-wall nanotubes of varying dimension. The relative intensity of the perturbed N2 mode tracks the cryogenic volumetric adsorption isotherms; as the spectroscopic probe can be completed in a few hours for a few micrograms of sample, the spectroscopic method provides a rapid screening alternative. Moreover, the spectroscopic probe elucidates site-specific interactions, which may advance the understanding of adsorbent geometry and chemical functionality, beyond that possible from deconstruction of bulk gas adsorption isotherms.

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