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Optimum Yield of the Purely Heterogeneous Oxidative Dimerization of Methane

Colussi, A. J. and Amorebieta, V. T. (1997) Optimum Yield of the Purely Heterogeneous Oxidative Dimerization of Methane. Journal of Catalysis, 169 (1). pp. 301-306. ISSN 0021-9517. https://resolver.caltech.edu/CaltechAUTHORS:20150623-154802540

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Abstract

The optimal C_2-yield per pass for the purely heterogeneous catalytic oxidation of methane by O_2 on Sm_2O_3 under continuous cofeed operation: η_(opt) ≤ 0.22 ± 0.03, is computed from actual kinetic data for all the pseudoelementary chemical reactions involved. The optimization dispenses with adjustable kinetic parameters, and explores the combined effects of CH_4 and O_2 flow rates, catalyst mass, residence time, and temperature variations on the objective function η = methane conversion × C_2-selectivity for the scheme: CH_4 (+O_2) ⇒ CH_3(→) 1/2 C_2H_6⇒ 1/2 C_2H_4⇒ CO. The fact that the derived η_(opt) value essentially coincides with the largest C_2-yields reported on a myriad catalysts under vastly different conditions: (1) proves that the ceiling to selectivity is solely determined by the competition among heterogeneous processes and (2) implies a substrate-independent selectivity pattern for the species formed in O_2 dissociative chemisorption. We briefly analyze the physical basis of these propositions and of the prospects of improving C_2-yields beyond 25%.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1006/jcat.1997.1678DOIArticle
http://www.sciencedirect.com/science/article/pii/S002195179791678XPublisherArticle
ORCID:
AuthorORCID
Colussi, A. J.0000-0002-3400-4101
Additional Information:© 1997 Academic Press. Received November 26, 1996; revised February 28, 1997; accepted March 3, 1997. This project was financially supported by CONICET/Argentina under Grant PID1131/91.
Funders:
Funding AgencyGrant Number
Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET)PID1131/91
Issue or Number:1
Record Number:CaltechAUTHORS:20150623-154802540
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150623-154802540
Official Citation:A.J. Colussi, V.T. Amorebieta, Optimum Yield of the Purely Heterogeneous Oxidative Dimerization of Methane, Journal of Catalysis, Volume 169, Issue 1, 1 July 1997, Pages 301-306, ISSN 0021-9517, http://dx.doi.org/10.1006/jcat.1997.1678. (http://www.sciencedirect.com/science/article/pii/S002195179791678X)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:58501
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:29 Jul 2015 21:54
Last Modified:03 Oct 2019 08:36

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