Editors: | Vayenas Intl. Symp. / Physical Chemistry and its applications for sustainable development Edited by: F. Kongoli, E. Aifantis, C. Cavalca, A. de Lucas Consuegra, A. Efstathiou, M. Fardis, D. Grigoriou, A. Lemonidou, S.G. Neophytides, Y. Roman, M. Stoukides, M. Sullivan, P. Vernoux, X. Verykios, I. Yentekakis |
Publisher: | Flogen Star OUTREACH |
Publication Year: | 2019 |
Pages: | 249 pages |
ISBN: | 978-1-989820-09-4 |
ISSN: | 2291-1227 (Metals and Materials Processing in a Clean Environment Series) |
During the last decades, several natural gas (NG) reservoirs were found to be rich in CO2 (> 40 vol%), and this led to an intense effort for the development of a dry reforming of methane (DRM) catalytic technology (CH4 + CO2 to 2 CO + 2 H2) with a favorable H2/CO gas ratio for liquid fuels (Gas To Liquid, GTL) and other useful chemicals (e.g., DME, MeOH, acetic acid) by the catalysis research community and related industries [1]. Biogas (a renewable energy source) can also be a suitable feedstock for the DRM catalytic technology [2].
Practical problems related to the irreversible coking phenomena, especially on the less-costly attractive Ni-based catalysts, remain one of the main obstacles for the catalytic DRM technology to find industrial applications. It is well known that an in-depth understanding of the elementary steps related to carbon deposition and removal chemistry on Ni or other relevant metal supported catalytic systems along with their micro-kinetic analysis is a key factor for the future development of highly active and
carbon - resistant DRM catalytic systems, preferably at temperatures lower than 750 oC.
This keynote lecture will present the use of various transient and isotopic experiments (use of 18O2, 13CO2 and 13CH4) to elucidate the role of metal cation dopant in Ce1-xMxO2 (M = Ti4+, Pr3+) used as support of Ni, and the use of Pt in the NiPt alloy supported on Ce0.8Pr0.2O2, in reducing the carbon accumulation to a remarkable extent during DRM at 750oC. In particular, the importance of carbon gasification by labile oxygen of support to the formation of CO(g), the contribution of oxygen vacant sites of support to the CO2 dissociation rate and re-oxidation of support, and the quantification of the origin of carbon accumulation (CH4 vs CO2 activation route) will be elucidated [3, 4]. Other experimental approaches reported in the literature for the understanding of carbon deposition and removal chemistry on supported Ni and other metals will be presented. Experimental results from the SSITKA technique (use of 13CO2 or 13CH4) will be presented to demonstrate the effect of metal dopant on support and Pt on the active carbon that is strictly associated with the rate of reaction.