On the coke deposition in dry reforming of methane at elevated pressures

Autor: Linus Schulz, Olaf Deutschmann, Stephan Andreas Schunk, Lea C. S. Kahle, Johannes A. Lercher, Andreas Jentys, Karla Herrera Delgado
Rok vydání: 2015
Předmět:
Zdroj: Applied Catalysis A: General. 504:599-607
ISSN: 0926-860X
DOI: 10.1016/j.apcata.2015.03.002
Popis: The reaction pathways leading to coke formation in dry reforming on Ni and Pt-based catalysts were investigated. Using isotope-labeled reactants (i.e., CH 4 + 13 CO 2 ⇌ 2CO + 2H 2 ) showed that initially 13 CO 2 is converted faster than CH 4 and that this higher activity leads to a higher concentration of 13 CO compared with 12 CO in the product stream, suggesting little isotope scrambling among products at this stage. Gasification of carbon deposits was found to be an important pathway enhancing the catalyst stability. Analysis of the pathways leading to carbon deposits suggests that coke is formed predominantly via reverse Boudouard reaction on Ni, while both metals contribute to CH 4 dissociation. The pronounced reversibility of the C H and C O bond formation and cleavage was also shown by the presence of 13 CH 4 formed from 13 CO 2 and 12 CO formed from 12 CH 4 . Numeric calculations complementing the experimental results led to the proposal of a reaction pathway for the surface reactions, accounting for the differences between Ni and Pt.
Databáze: OpenAIRE