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Effect of syngas conversion and catalyst reduction temperature in the synthesis of ethanol: concentration of water vapor in mesoporous Rh/MCM-41 catalyst
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology. UMSA Universidad Mayor de San Andres, Bolivia.ORCID iD: 0000-0001-8488-4429
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.ORCID iD: 0000-0002-3793-1197
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
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2015 (English)In: Catalysis communications, ISSN 1566-7367, E-ISSN 1873-3905, Vol. 69, 183-187 p.Article in journal (Refereed) Published
Abstract [en]

Rh-based catalysts typically show low selectivity to CO2 in the synthesis of ethanol from syngas. However, a novel mesoporous Rh/MCM-41 catalyst shows high selectivity to CO2 in a large range of syngas conversions; 1% to 68%, regulated by adjusting the operation conditions (270-430 degrees C, 30-90 bar and 6000-40,000 ml(syngas)/gcat h). The same effect is obtained at different catalyst reduction temperatures (200 degrees C and 500 degrees C) as well as on the non-reduced catalyst. A high concentration of water vapor seems to occur in the pores of Rh/MCM-41 which may promote the water-gas-shift-reaction, producing extra CO2 and H-2. (C) 2015 Elsevier B.V. All rights reserved.

Place, publisher, year, edition, pages
Elsevier, 2015. Vol. 69, 183-187 p.
Keyword [en]
Ethanol, Reduction temperature, Rh/MCM-41, Syngas conversion
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-173417DOI: 10.1016/j.catcom.2015.06.015ISI: 000359885900039Scopus ID: 2-s2.0-84934278111OAI: oai:DiVA.org:kth-173417DiVA: diva2:853964
Funder
Sida - Swedish International Development Cooperation Agency
Note

QC 20150915

Available from: 2015-09-15 Created: 2015-09-11 Last updated: 2017-12-04Bibliographically approved
In thesis
1. Catalytic conversion of syngas to ethanol and higher alcohols over Rh and Cu based catalysts
Open this publication in new window or tab >>Catalytic conversion of syngas to ethanol and higher alcohols over Rh and Cu based catalysts
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The thermochemical process converts almost any kind of biomass to a desired final product, i.e. gaseous or liquid transportation fuels and chemicals. The transportation fuels obtained in this way are renewable biofuels, which are alternatives to fossil fuels. During the last few years, thermochemical plants for the production of bioethanol have been launched and another is under construction. A total of about 290 million liters of ethanol are expected to be processed per year, mostly using municipal solid waste. Considerable efforts have been made in order to find a more selective catalyst for the conversion of biomass-derived syngas to ethanol.

The thesis is the summary of five publications. The first two publications (Papers I and II) review the state of the art of ethanol and higher alcohols production from biomass, as well as the current status of synthetic fuels production by other processes such as the Fischer-Tropsch synthesis. Paper III analyses the catalytic performance of a mesoporous Rh/MCM-41 (MCM-41 is a hexagonal mesoporous silica) in the synthesis of ethanol which is compared to a typical Rh/SiO2 catalyst. Exhaustive catalytic testing including the addition of water vapor and modifying the hydrogen partial pressure in the syngas feed-stream which, in addition to the catalyst characterization (XRD, BET, XPS, chemisorption, TEM and TPR) before and after the catalytic testing, have allowed concluding that some water vapor can be concentrated in the pores of the Rh/MCM-41 catalyst. The concentration of water-vapor promotes the occurrence of the water gas shift reaction, which in turn induces some secondary reactions that change the product distribution, as compared to results obtained from the typical Rh/SiO2 catalyst. These results have been verified in a wide range of syngas conversion levels (1-68 %) and for different catalyst activation procedures (catalyst reduction at 200 °C, 500 °C and no-reduction) as shown in Paper IV. Finally, similar insights about the use of mesoporous catalyst have been found over a Cu/MCM-41 catalyst, shown in Paper V. Also in Paper V, the effect of metal promoters (Fe and K) has been studied; a noticeable increase of ethanol reaction rate was found over Cu-Fe-K/MCM-41 catalyst as compared to Cu/MCM-41. 

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2017. 98 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2017:2
Keyword
thermochemical process, ethanol, higher alcohols, mesoporous catalysts, rhodium, copper, metal promoters
National Category
Chemical Engineering
Research subject
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-196808 (URN)978-91-7729-206-7 (ISBN)
Public defence
2017-01-27, Q2, Osquldas väg 10, Våning 2, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Sida - Swedish International Development Cooperation Agency
Note

QC 20161125

Available from: 2016-11-25 Created: 2016-11-22 Last updated: 2017-02-03Bibliographically approved

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Velasco, Jorge A.

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