One‐step catalytic conversion of ethanol to butadiene in the fixed bed. I. Single‐oxide catalysts

Bhattacharyya, S. K.; Ganguly, N.D.

doi:10.1002/jctb.5010120301

Cited by 27 publications

(19 citation statements)

References 3 publications

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“…Apart from the review of those listed, the published literature on the one-step catalytic conversion is meager. While single, binary and ternary-oxide catalyst systems are all used in this field, such as Al 2 [9,[13][14][15][16][17][18][19] and so on, and the process of ethanol conversion to BD is similar.…”

Section: Introductionmentioning

confidence: 98%

Study on the Mechanism of Butadiene Formation from Ethanol

et al. 2014

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An specific investigation has been carried out on the mechanism of the catalytic conversion of ethanol to 1,3-butadiene on magnesia-silica acidic-basic bifunctional catalysts. The magnesia-silica catalyst was prepared by wet-kneading and the reaction process was detected through Impulse Response and Diffuse Reflectance Infrared Fourier Transform Spectroscopy. The mechanism of 1,3-butadiene formation from ethanol was demonstrated through experiment in this time, and the process was proved as follows: Firstly, ethanol was dehydrogenated to form acetaldehyde; Then condensation of acetaldehyde formed acetaldol; Then dehydration of acetaldol to croton aldehyde; Finally, ethanol was involved a second time in a hydrogen transfer reaction with croton aldehyde to form 1,3-butadiene.

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Section: Introductionmentioning

confidence: 98%

Study on the Mechanism of Butadiene Formation from Ethanol

et al. 2014

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“…Usually, enhancement of 1,3-BD selectivities [13,19] and yields [19,27] could be observed when the WHSV was reduced, suggesting the positive effect of contact times on reaction yields, as one might already expect. However, nonlinear effects of ethanol flow rates on 1,3-BD yields were verified over different single and binary metal oxides (such as MgO, ZrO2, Al2O3-MgO, Al2O3-Fe2O3, Al2O3-Cr2O3 and ZrO2-Fe2O3) [30,31].…”

Section: Introductionmentioning

confidence: 98%

“…Usually, reaction variables are investigated using the "change-one-factor-at-atime" method; that is, one variable is changed while the other experimental conditions are kept constant [2,10,12,13,26,27,[29][30][31]. Based on this method, it has been found that temperature exerts an important nonlinear effect on 1,3-BD yields, as observed with help of different catalysts [13,19,26,30,31]. Similar studies have shown that the weight hourly space velocity (WHSV) also modifies 1,3-BD yields and selectivities [2,13,19,26,27,30,31].…”

Section: Introductionmentioning

confidence: 99%

“…Based on this method, it has been found that temperature exerts an important nonlinear effect on 1,3-BD yields, as observed with help of different catalysts [13,19,26,30,31]. Similar studies have shown that the weight hourly space velocity (WHSV) also modifies 1,3-BD yields and selectivities [2,13,19,26,27,30,31]. Usually, enhancement of 1,3-BD selectivities [13,19] and yields [19,27] could be observed when the WHSV was reduced, suggesting the positive effect of contact times on reaction yields, as one might already expect.…”

Section: Introductionmentioning

confidence: 99%

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Modelling the effects of reaction temperature and flow rate on the conversion of ethanol to 1,3-butadiene

Ros

Jones

Mattia

et al. 2017

Applied Catalysis A: General

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A full factorial experimental design was performed to investigate the conversion of ethanol to 1,3-butadiene (1,3-BD), through manipulation of the reaction temperature and ethanol weight hourly space velocity. Reactions were carried out in presence of the catalyst K2O:ZrO2:ZnO/MgO-SiO2, prepared by co-precipitation methods. Mathematical models were developed to correlate observed product selectivities, 1,3-BD yields and productivities with the manipulated reaction variables, allowing for quantification of variable effects on catalyst activity and assessment of the kinetic mechanism. Obtained 1,3-BD productivities were as high as 0.5 gBD/gcat.h, with 1,3-BD yields of 27 %. Results suggest that acetaldehyde condensation is the rate determining step.

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“…~70% yield [19]. In general, doped-MgO supported on silica [18,[20][21][22][23][24][25][26][27][28][29]] (Lebedev's catalyst) or mixed (supported) oxides [16,19,[30][31][32][33][34][35][36] were used. Various transition metal dopants (Zn, Cu, and Ag) were used to improve MgO/SiO 2 catalyst performance, as well as different synthesis methods and composition of MgO/SiO 2 were investigated, such as Kvisle's wet kneading method [26] and the utilization of clay and sepiolite as the support [21,28].…”

Section: Introductionmentioning

confidence: 99%

Catalytic conversion of ethanol to 1,3-butadiene on MgO: A comprehensive mechanism elucidation using DFT calculations

Taifan

Bučko

Baltrušaitis

2017

Journal of Catalysis

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In this work, we performed periodic Density Functional Theory calculations and explored reactive pathways of ethanol catalysis to catalytically form 1,3-butadiene on undoped MgO surface. We have identified critical reactive intermediates, as well as thermodynamic and kinetic barriers involved in the overall reactive landscape. The overall free energy surface was explored for the highly debated reaction mechanisms, including Toussaint's aldol condensation mechanism, Fripiat's Prins mechanism and mechanism based on Ostromislensky's hemiacetal rearrangement. Thermodynamics and kinetics data calculated showed four rate limiting steps in the overall process. In particular, ethanol dehydration to form ethylene possessed lower energy barrier than dehydrogenation to yield acetaldehyde suggesting competing reactive pathways. CC bond coupling to form acetaldol (3-hydroxybutanal) is preceded with 16 kcal/mol forward reaction barrier. Direct reaction of ethylene and acetaldehyde proceeds with a free energy barrier of 29 kcal/mol suggesting that Prins condensation is an alternative route. Finally, thermodynamic stability of 1-ethoxyethanol prevents further reaction via hemiacetal rearrangement. The results here provide a first glimpse into the overall 1,3-butadiene formation mechanism on undoped MgO reactive sites in light of the vast literature discussing variety of the proposed mechanistic pathways mostly based on conventional homogenous organic chemistry reactions.

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One‐step catalytic conversion of ethanol to butadiene in the fixed bed. I. Single‐oxide catalysts

Cited by 27 publications

References 3 publications

Study on the Mechanism of Butadiene Formation from Ethanol

Study on the Mechanism of Butadiene Formation from Ethanol

Modelling the effects of reaction temperature and flow rate on the conversion of ethanol to 1,3-butadiene

Catalytic conversion of ethanol to 1,3-butadiene on MgO: A comprehensive mechanism elucidation using DFT calculations

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