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Catalytic conversion of syngas to higher alcohols over MoS 2 -based catalysts [Elektronisk resurs]

Andersson, Robert (författare)
Boutonnet, Magali (preses)
Järås, Sven (preses)
Holmen, Anders (opponent)
KTH Skolan för kemivetenskap (CHE) (utgivare)
Publicerad: Stockholm : KTH Royal Institute of Technology, 2015
Engelska ix, 106
Serie: TRITA-CHE-Report, 1654-1081
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  • E-bokAvhandling(Diss. (sammanfattning) Stockholm : Kungliga Tekniska högskolan, 2015)
Sammanfattning Ämnesord
Stäng  
  • The present thesis concerns catalytic conversion of syngas (H 2 + CO) into a blend of methanol and higher alcohols, an attractive way of producing fuels and chemicals. This route has the potential to reduce the oil dependence in the transport sector and, with the use of biomass for the syngas generation, produce CO 2 -neutral fuels. Alkali promoted MoS 2 -based catalysts show a high selectivity to higher alcohols, while at the same time being coke resistant, sulfur tolerant and displaying high water-gas shift activity. This makes this type of catalyst especially suitable for being used with syngas derived from biomass or coal which typically has a low H 2 /CO-ratio. This thesis discusses various important aspects of higher alcohol synthesis using MoS 2 -based catalysts and is a summary of four scientific papers. The first part of the thesis gives an introduction to how syngas can be produced and converted into different fuels and chemicals. It is followed by an overview of higher alcohol synthesis and a description of MoS 2 -based catalysts. The topic alcohol for use in internal combustion engines ends the first part of the thesis. In the second part, the experimental part, the preparation of the MoS 2 -based catalysts and the characterization of them are handled. After describing the high-pressure alcohol reactor setup, the development of an on-line gas chromatographic system for higher alcohol synthesis with MoS 2 catalysts is covered (Paper I). This method makes activity and selectivity studies of higher alcohol synthesis catalysts more accurate and detailed but also faster and easier. Virtually all products are very well separated and the established carbon material balance over the reactor closed well under all tested conditions. The method of trace level sulfur analysis is additionally described. Then the effect of operating conditions, space velocity and temperature on product distribution is highlighted (Paper II). It is shown that product selectivity is closely correlated with the CO conversion level and why it is difficult to combine both a high single pass conversion and high alcohol selectivity over this catalyst type. Correlations between formed products and formation pathways are additionally described and discussed. The CO 2 pressure in the reactor increases as the CO conversion increases, however, CO 2 influence on formation rates and product distribution is to a great extent unclear. By using a CO 2 -containing syngas feed the effect of CO 2 was studied (Paper III). An often emphasized asset of MoS 2 -based catalysts is their sulfur tolerance. However, the use of sulfur-containing feed and/or catalyst potentially can lead to incorporation of unwanted organic sulfur compounds in the product. The last topic in this thesis covers the sulfur compounds produced and how their quantity is changed when the feed syngas contains H 2 S (Paper IV). The effect on catalyst activity and selectivity in the presence of H 2 S in the feed is also covered. 

Ämnesord

Engineering and Technology  (hsv)
Chemical Engineering  (hsv)
Teknik och teknologier  (hsv)
Kemiteknik  (hsv)
Chemical Engineering  (kth)
Kemiteknik  (kth)

Indexterm och SAB-rubrik

conversion
higher alcohols
mixed alcohols
MoS2
syngas
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