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Synthesis gas production for GTL applications: Thermodynamic equilibrium approach and potential for carbon formation in a catalytic partial oxidation pre-reformer
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology. UMSA - Universidad Mayor de San Andrés, Bolivia.ORCID iD: 0000-0002-3793-1197
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology. UMSA - Universidad Mayor de San Andrés, Bolivia.ORCID iD: 0000-0001-8488-4429
UMSA - Universidad Mayor de San Andrés, Bolivia.
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
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2014 (English)In: Journal of Natural Gas Science and Engineering, ISSN 1875-5100, E-ISSN 2212-3865, Vol. 20, 175-183 p.Article in journal (Refereed) Published
Abstract [en]

The present work is focused on synthesis gas production for Gas to Liquids (GTL.) applications. A thermodynamic equilibrium approach has been chosen in order to address the methane reforming processes in presence of steam and oxygen (i.e. autothermal reforming "ATR" and catalytic partial oxidation "CPO"). The effect of operational variables on the performance of the reforming units has been analyzed at conditions typical for GTL processes. Also, the performance of a synthesis gas generation unit (SGU) comprising a CPO pre-reformer followed by an ATR reactor has been investigated. The potential for carbon formation in the CPO pre-reformer has been evaluated by applying the "equilibrated gas principle". Our results show that synthesis gas production can be strongly influenced by changes in operating variables such as the steam-to-carbon (S/C) and the oxygen-to-carbon (O-2/C) ratios, recycled gas (tail gas) compositions, and operating pressures and temperatures; however, effective operation of the SGU (CPO + ATR) requires an correct combination of these variables in order to accomplish the synthesis gas requirements of the Fischer-Tropsch synthesis. Likewise, it is shown that the risk of carbon formation in the CPO reactor can be reduced or even eliminated by a proper manipulation and combination of such variables.

Place, publisher, year, edition, pages
Elsevier, 2014. Vol. 20, 175-183 p.
Keyword [en]
Catalytic partial oxidation, Equilibrated gas principle, GTL applications, Synthesis gas production, Thermodynamic equilibrium
National Category
Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-154767DOI: 10.1016/j.jngse.2014.06.021ISI: 000342258100021Scopus ID: 2-s2.0-84904318902OAI: oai:DiVA.org:kth-154767DiVA: diva2:760655
Funder
Sida - Swedish International Development Cooperation Agency
Note

QC 20141104

Available from: 2014-11-04 Created: 2014-10-27 Last updated: 2017-12-05Bibliographically 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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