Title

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.

Department(s)

Chemical and Biochemical Engineering

Sponsor(s)

United States. Department of Energy. Office of Basic Energy Sciences

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.

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.

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