Spectroscopic identification of hydrogen spillover species in ruthenium-modified high surface area carbons by diffuse reflectance infrared fourier transform spectroscopy

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dc.contributor.authorBlackburn, JLen_AU
dc.contributor.authorEngtrakul, Cen_AU
dc.contributor.authorBult, JBen_AU
dc.contributor.authorHurst, Ken_AU
dc.contributor.authorZhao, Yen_AU
dc.contributor.authorXu, Qen_AU
dc.contributor.authorParilla, PAen_AU
dc.contributor.authorSimpson, LJen_AU
dc.contributor.authorRocha, JDRen_AU
dc.contributor.authorHudson, MRen_AU
dc.contributor.authorBrown, CMen_AU
dc.contributor.authorGennett, Ten_AU
dc.date.accessioned2013-09-25T06:06:52Zen_AU
dc.date.available2013-09-25T06:06:52Zen_AU
dc.date.issued2012-12-27en_AU
dc.date.statistics2013-09-25en_AU
dc.description.abstractIn recent years, carbon-based sorbents have been recognized for their potential application within vehicular hydrogen storage applications. One method by which sorbents have been reported to store appreciable hydrogen at room temperature is via a spillover process: where molecular hydrogen is first dissociated by metal nanoparticle catalysts and atomic hydrogen subsequently migrates onto the carbon substrate. Many reports have invoked the spillover mechanism to explain enhancements in reversible room temperature hydrogen uptake for metal-decorated sorbents. However, there is a lack of experimental evidence for the proposed chemical species formed as well as several differing theoretical explanations describing the process. In this report, we utilize diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to identify the various chemical species formed upon room temperature H-2 charging of ruthenium-decorated high surface area carbons. Room temperature H-2 loading of a control sample with no ruthenium nanoparticles (Ru NPs) leads to broad reversible peaks in the DRIFTS spectrum that correspond to the vibration-rotation transitions of weakly bound physisorbed hydrogen molecules. In contrast, the sample modified with Ru NPs shows a variety of reversible and irreversible peaks in addition to the physisorbed H-2 peaks. Rigorous experimental and theoretical analysis enables the assignment of the peaks to ruthenium-mediated formation of water, surface hydroxyl groups (R-OH, where R = carbon or ruthenium), and C-H bonds. The low-energy DRIFTS peaks assigned to spillover C-H bonds were additionally confirmed using inelastic neutron spectroscopy. Reversible vibrational peaks consistent with ruthenium-mediated formation of C-H bonds provide much-needed spectroscopic evidence for the spillover process. The results demonstrated here should facilitate future mechanistic investigations of hydrogen sorption on transition metal nanoparticles and high surface area activated carbons. © 2012, American Chemical Society.en_AU
dc.identifier.citationBlackburn, J. L., Engtrakul, C., Bult, J. B., Hurst, K., Zhao, Y., Xu, Q., Parilla, P. A., Simpson, L. J., Rocha, J. D. R., Hudson, M. R., Brown, C. M., & Gennett, T. (2013). Spectroscopic identification of hydrogen spillover species in ruthenium-modified high surface area carbons by diffuse reflectance infrared fourier transform spectroscopy. Journal of Physical Chemistry C, 116 (51), 26744-26755. doi:10.1021/jp305235pen_AU
dc.identifier.govdoc5139en_AU
dc.identifier.issn1932-7447en_AU
dc.identifier.issue51en_AU
dc.identifier.journaltitleJournal of Physical Chemistry Cen_AU
dc.identifier.pagination26744-26755en_AU
dc.identifier.urihttp://dx.doi.org/10.1021/jp305235pen_AU
dc.identifier.urihttp://apo.ansto.gov.au/dspace/handle/10238/4741en_AU
dc.identifier.volume116en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Society.en_AU
dc.subjectNeutronsen_AU
dc.subjectScatteringen_AU
dc.subjectCarbonen_AU
dc.subjectHydrogenen_AU
dc.subjectRutheniumen_AU
dc.subjectSorptionen_AU
dc.titleSpectroscopic identification of hydrogen spillover species in ruthenium-modified high surface area carbons by diffuse reflectance infrared fourier transform spectroscopyen_AU
dc.typeJournal Articleen_AU
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