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Methane partial oxidation and methane decomposition over Ni andNi-Ru supported catalysts for synthesis gas production
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.ORCID iD: 0000-0002-3793-1197
Organic Chemistry Department, University of Córdoba, Córdoba, Spain.
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
Instituto del Gas Natural, San Andrés Higher University, La Paz, Bolivia.
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Nickel and nickel-ruthenium based catalysts were compared in the catalytic partial oxidation (CPO) of methane and in the equilibrium of the methane decomposition reaction. A hydrotalcite-derived material as well as α- Al2O3 and γ-Al2O3 were used as catalyst supports. The catalysts were characterized by H2 chemisorption, N2 physisorption, temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO) and transmission electron microscopy (TEM). Catalyst properties and composition influenced the catalytic performance during partial oxidation (i.e. activity and temperature profiles). During methane decomposition equilibrium tests, all catalysts presented smaller equilibrium constants than those calculated on the basis of graphite; the deviation from graphite data was mainly associated with maximum nickel particle size (for both Ni and bimetallic Ni-Ru supported catalysts). Among all catalysts, the bimetallic Ni-Ru catalyst supported on hydrotalcite-derived material showed an interesting enhanced behavior; however, resistance towards catalyst deactivation, by mechanisms different than carbon formation, still needs to be improved. 

Keyword [en]
carbon formation, methane decomposition, nickel, partial oxidation of methane, ruthenium, synthesis gas
National Category
Chemical Process Engineering
Research subject
Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-176409OAI: oai:DiVA.org:kth-176409DiVA: diva2:866800
Note

QS 2015

Available from: 2015-11-03 Created: 2015-11-03 Last updated: 2015-11-04Bibliographically approved
In thesis
1. Catalytic partial oxidation of methane over nickel and ruthenium based catalysts for GTL applications
Open this publication in new window or tab >>Catalytic partial oxidation of methane over nickel and ruthenium based catalysts for GTL applications
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The Gas to Liquids (GTL) process is an important alternative for monetizing natural gas through the production of long-chain liquid hydrocarbons, e.g. diesel fuel. The GTL process involves three main steps: synthesis gas production to obtain H2 and CO, Fischer-Tropsch synthesis to obtain a synthetic crude oil, and upgrading/refining to obtain final products. Since the synthesis gas production is the most expensive step, there is great interest in optimizing and exploring new routes for syngas production.

This thesis focuses on the conversion of methane, the main component of natural gas, into synthesis gas by catalytic partial oxidation (CPO). Several aspects of the CPO reaction in the context of the GTL technology are discussed. The work contributes to an increased knowledge concerning utilizing a CPO reactor as pre-reformer in the synthesis gas production process as well as the influence of catalyst properties and composition on the catalytic behavior when using nickel and ruthenium-based catalysts in the CPO reaction.

The thesis is a summary of five publications. The first two publications (Papers I and II) review the current status of both the GTL technology and the catalytic partial oxidation of methane. Paper III analyzes a process configuration comprising of a CPO pre-reformer followed by an autothermal reforming (ATR) reactor using a thermodynamic equilibrium approach. It was found that a proper manipulation of the process conditions is needed to obtain a suitable synthesis gas for GTL applications simultaneously of minimizing the risk of carbon formation in the CPO reactor; the operation of the CPO reactor demanded low O2/CH4 and H2O/CH4 feed molar ratios. Accordingly, in paper IV, the partial oxidation of methane at low O2/CH4 and H2O/CH4 ratios is investigated over nickel and ruthenium catalysts supported on MgO/MgAl2O4 and compared with a commercial nickel-based catalyst. The extent or impact of the combustion and reforming reactions along the catalytic bed are substantially influenced by catalyst properties and composition. Deactivation by carbon formation is also discussed; ruthenium-containing catalysts might positively overcome carbon formation. To gain greater insight concerning the influence of the catalyst composition and properties on carbon formation, a set of nickel and bimetallic nickel-ruthenium catalysts, supported on α-Al2O3, γ-Al2O3 and MgO/MgAl2O4, is tested in the CH4 decomposition reaction in Paper V. For these catalysts, the resistance towards carbon formation is mainly correlated with the nickel particle size. 

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. xi, 83 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:63
Keyword
Catalytic partial oxidation, carbon formation, GTL, nickel, ruthenium, synthesis gas, thermodynamic equilibrium.
National Category
Chemical Engineering
Research subject
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-176424 (URN)978-91-7595-753-1 (ISBN)
Public defence
2015-11-27, K1, Teknikringen 56, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20151105

Available from: 2015-11-04 Created: 2015-11-03 Last updated: 2015-11-04Bibliographically approved

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Velasco, Jorge A.

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