Evidence for Ambient-Temperature Reversible Catalytic Hydrogenation in Pt-Doped Carbons
Abstract
In situ high-pressure Raman spectroscopy, with corroborating density functional calculations, is used to probe C-H chemical bonds formed when dissociated hydrogen diffuses from a platinum nanocatalyst to three distinct graphenic surfaces. At ambient temperature, hydrogenation and dehydrogenation are reversible in the combined presence of an active catalyst and oxygen heteroatoms. Hydrogenation apparently occurs through surface diffusion in a chemisorbed state, while dehydrogenation requires diffusion of the chemisorbed species back to an active catalyst.
Recommended Citation
X. Liu and Y. Tang and E. Xu and T. C. Fitzgibbons and G. S. Larsen and H. R. Gutierrez and H. Tseng and M. Yu and C. S. Tsao and J. V. Badding and V. H. Crespi and A. D. Lueking, "Evidence for Ambient-Temperature Reversible Catalytic Hydrogenation in Pt-Doped Carbons," Nano Letters, vol. 13, no. 1, pp. 137 - 141, American Chemical Society (ACS), Nov 2013.
The definitive version is available at https://doi.org/10.1021/nl303673z
Department(s)
Chemical and Biochemical Engineering
Sponsor(s)
United States. Department of Energy. Office of Basic Energy Sciences
Keywords and Phrases
Active catalyst; Catalytic hydrogenation; Graphane; Heteroatoms; Nano-catalyst; Pt nanoparticles; Spillover; Catalysis; Catalysts; Chemical bonds; Chemisorption; Dehydrogenation; Density functional theory; Graphene; Hydrogen; Platinum; Raman spectroscopy; Hydrogenation; Catalysis
International Standard Serial Number (ISSN)
1530-6984
Document Type
Article - Journal
Document Version
Citation
File Type
text
Language(s)
English
Rights
© 2013 American Chemical Society (ACS), All rights reserved.
Publication Date
01 Nov 2013
Comments
This work was supported by the U.S. Department of Energy, Basic Energy Sciences. The Raman, TEM, and DFT aspect of the work was supported under the Single Investigator and Small-Group Research (SISGR) program, Awards DE-FG02- 09ER466556 and DE-SC0002157. T.C.F. (providing Raman support and FTIR and Raman analysis) and J.V.B. were additionally supported as part of Energy Frontier Research in Extreme Environments Center (EFree), an Energy Frontier Research Center under Award No. DE-SC0001057. The adsorption isotherms referenced in this work were supported by the Energy Efficiency and Renewable Energy program, Award DE-FG36-08GO18139.