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Zharova P.A.,Av Topchuev Institute Of Petrochemical Synthesis | Chistyakov A.V.,Av Topchuev Institute Of Petrochemical Synthesis | Tsodikov M.V.,Av Topchuev Institute Of Petrochemical Synthesis | Nikolaev S.A.,Moscow State University | And 2 more authors.
Chemical Engineering Transactions | Year: 2016

The importance of synthesis of carbon-carbon bonds is reflected by the fact that Nobel Prizes in Chemistry have been given to this area: The Grignard reaction (1912), the Diels-Alder reaction (1950), the Witting reaction (1979), the olefin metathesis Y. Chauvin, R.H. Grubbs and R.R. Schrock (2005), the palladiumcatalyzed cross-coupling reactions to R. F. Heck, A. Suzuki, E. Negishi (2010). For the first time ever alkylation of isopropanol with ethanol was carried out over heterogeneous 0.2-1 wt.% Au and/or 0.02-0.3 wt. %Ni - containing catalysts without any sacrificial agents and/or presence of acidic/base additives. The catalyst containing 0.2 wt.% Au and 0.18 wt.% Ni supported on γ-Al2O3 was found to be the most selective in the cross-coupling route. Total selectivity of coupling products reached up to 70 %, conversion of the both initial alcohols was 50 %. Structural investigations of the Au, Ni - containing catalysts permitted to determine probable active sites peculiarities that provide effective one-pot alkylation of isopropanol with ethanol. Copyright © 2016, AIDIC Servizi S.r.l..


Tsodikov M.V.,Av Topchuev Institute Of Petrochemical Synthesis | Murzin V.Y.,Av Topchuev Institute Of Petrochemical Synthesis | Chistyakov A.V.,Av Topchuev Institute Of Petrochemical Synthesis | Yandieva F.A.,Av Topchuev Institute Of Petrochemical Synthesis | And 7 more authors.
Chemical Engineering Transactions | Year: 2014

Here, we present ethanol transformation into hydrocarbons C4-C12 through a one-step catalytic process. A number of industrial Pt-containing catalysts samples (AP-64, R-254, IP-62, Pt-Re/Al2O3) were used, as well as an original Pt-Sn/Al2O3 catalyst. All the catalytic experiments were carried out at 5 atm and 350°C. After a pretreatment procedure under 50 atm of H2 at 450 °C during 12 hours, the catalysts improved a enhanced selectivity to hydrocarbons. After about 10 hours on stream, catalytic activity decreased due to coking issues. However, high catalytic performance could be recovered after calcination in air followed by reduction at 450 °C. In general, the hydrocarbons C4-C12 yield varied from 20 to 50 wt.% over the different catalysts samples. Depending on the support nature, the ethanol was preferentially converted to alkanes or olefins. The effect of metal addition to Pt-containing catalysts was studied on some industrial Pt-Re and one original Pt-Sn samples. Re addition led to high activity for the formation of olefins, of which the yield reached up to 40 wt.%. Sn addition promoted both olefins and oxygenates formation. The most suitable catalyst for obtaining fuel hydrocarbons (gasoline compounds) was found to be the platinum/alumina catalyst AP-64. The structural particularities of this sample were studied using the XAS technique. Relations between the Pt clusters structure and the catalytic properties were identified. Copyright © 2014,AIDIC Servizi S.r.l.


Chistyakov A.V.,Av Topchuev Institute Of Petrochemical Synthesis | Murzin V.Yu.,Av Topchuev Institute Of Petrochemical Synthesis | Gubanov M.A.,Av Topchuev Institute Of Petrochemical Synthesis | Tsodikov M.V.,Av Topchuev Institute Of Petrochemical Synthesis
Chemical Engineering Transactions | Year: 2013

Development of the alternative hydrocarbon fuel sources is an urgent task in the current energy field. Ethanol can be considered as alternative basis for hydrocarbon fuel production. In this work we studied ethanol conversion into alkanes-olefines and alkane-aromatic hydrocarbons over palladium and zinc containing catalysts supported on alumina or MFI/alumina and mentioned catalysts structure, to give a reasonable explanation of the catalysts action mechanism. The catalyst based on MFI/alumina showed high stability to coking and stable productivity for over 48 hours. The total yield of the target fraction of C3- C12 hydrocarbons achieves 95 wt.% based on carbon. Among the obtained alkanes branched structures predominate. Copyright © 2013, AIDIC Servizi S.r.l.


Chistyakov A.V.,Av Topchuev Institute Of Petrochemical Synthesis | Gubanov M.A.,Av Topchuev Institute Of Petrochemical Synthesis | Tsodikov M.V.,Av Topchuev Institute Of Petrochemical Synthesis
Chemical Engineering Transactions | Year: 2013

The current study presents rapeseed oil conversion investigation over industrial Pt/γ-Al2O3 and Pd- Zn/MFI/γ-Al 2O3 catalysts. During reductive pre-treatment of Pt/γ-Al2O3 catalyst got new properties that results in the direct hydrogenative treatment of rape seed oil towards alkanes with total yield reached up to 90 wt.% and conversion about 100%. Via temperature varying one may adjust process selectivity towards hydrocarbons either gasoline or diesel fractions. It's noteworthy that initial oil contained acids with carbon number not exceeds 22, but products composition contained alkanes C 23+. The total yield of extra heavy alkanes C23+ was 0.5-5 wt.% depending on process conditions. Obtained data suggested the possibility of intermolecular cross-coupling reaction of glycerol fragments with acid fragments took place. Copyright © 2013, AIDIC Servizi S.r.l.


Chistyakov A.V.,Av Topchuev Institute Of Petrochemical Synthesis | Gubanov M.A.,Av Topchuev Institute Of Petrochemical Synthesis | Zharova P.A.,Av Topchuev Institute Of Petrochemical Synthesis | Tsodikov M.V.,University of Lille Nord de France | And 2 more authors.
Chemical Engineering Transactions | Year: 2014

The present study presents combined ethanol and rapeseed oil conversion to C4-C12 hydrocarbons via a one-step hydrogen-free catalytic process. As a catalyst an industrial Pd-Zn/Al2O3/MFI sample was used. The novelty of the suggested process resides in the combined conversion of rapeseed oil and ethanol (fermentation mixtures) in an inert atmosphere without external molecular hydrogen that is usually used for vegetable oils conversion. Our previous study showed that ethanol conversion over the Pd-Zn/Al2O3/MFI catalyst led to the formation of a surplus amount of hydrogen (Chistyakov et al., 2013a) that may be used for hydrogenolysis of the C-O bonds of fatty acids triglycerides during the combined conversion. In this work shown that the combined conversion produced significantly larger amounts of olefins and aromatics in comparison with conversion of pure ethanol. It is also shown that an initial concentration of 25-50 % of ethanol in the feed is optimal for the combined conversion. This amount of alcohol is sufficient to donate enough hydrogen to the system during conversion for a stable and smooth catalyst work while preventing coke formation. Fermentation mixtures and fusel oils were used for the combined conversion with rapeseed oil as well as ethanol. Copyright © 2014,AIDIC Servizi S.r.l.

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