Successive vapour phase Guerbet condensation of ethanol and 1-butanol over Mg-Al oxide catalysts in a flow reactor

Larina, Olga V.; Valihura, Karina V.; Kyriienko, Pavlo I.; Vlasenko, N. A.; Balakin, Dmytro Yu.; Khalakhan, Ivan; Čendak, Tomaž; Soloviev, Sergiy O.; Orlyk, S. M.

doi:10.1016/j.apcata.2019.117265

Cited by 43 publications

(29 citation statements)

References 43 publications

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“…Non‐oxidative thermocatalytic conversion of ethanol on a monometallic low‐percentage Cu/ γ ‐Al 2 O 3 catalyst includes the parallel formation of ethylene, acetaldehyde, and gaseous products (CH 4 , CO 2 , CO, H 2 ) through dehydration, dehydrogenation, and decomposition of ethanol, respectively 58–60 (Scheme 1). For the monometallic catalyst, the selectivity to unwanted products was the highest.…”

Section: Resultsmentioning

confidence: 99%

Effect of Ni, La, and Ce Oxides on a Cu/Al₂O₃ Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

et al. 2021

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The effect of modifying additives (Ni, La, Ce oxides) on the activity of Cu/Al2O3 with a low copper loading was studied for ethanol non‐oxidative dehydrogenation. The catalysts were prepared by impregnation of the commercial Al2O3 granules and characterized by Brunauer‐Emmett‐Teller (BET), scanning electron microscopy (SEM), temperature‐programmed desorption of NH3 (TPD‐NH3), temperature‐programmed reduction of H2 (H2‐TPR), and thermogravimetric analysis (TGA). Modification of Cu/Al2O3 with Ni, La, and Ce oxides results in increasing catalytic activity. A modification of the Cu/Al2O3 catalyst with nickel and lanthanum oxides, in contrast to cerium oxide, leads to an improvement in the dispersion of the catalyst particles. The Cu‐Ni/Al2O3 catalyst with the highest acidity has the highest selectivity for acetaldehyde. The highest selectivity for butanol is observed for the Cu‐La/Al2O3 catalyst, which has the lowest acidity.

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Section: Resultsmentioning

confidence: 99%

Effect of Ni, La, and Ce Oxides on a Cu/Al₂O₃ Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

et al. 2021

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“…So, acetaldehyde is considered as an intermediate of reaction (indirect route), generated both by the non-oxidative dehydrogenation on basic-sites preferentially Ca-O-Ca centers 25 Modeling and Analysis: Understanding the biobutanol production process or by the decomposition of surface ethoxide-species; considering that the amount of basic sites is enough to carry out the reaction, the differences in the product distribution would be associated with the presence of acid-base cooperative centers. 53 The formation of n-butanol would be promoted by those catalysts able to stabilize the adsorbed acetaldehyde and by self-condensation involving Ca-O-P and Ca-O-Al sites 26,28,54 to form acetaldol (3-hydrobutanal) or the carbanion formed upon ethanol adsorption on catalyst; however the aldol-condensation (ethanol and acetaldehyde) will promote the butene species that were not detected for these model catalysts and the stabilization of carbanion would favor ethylene and DEE production in acid sites. Besides, crotyl alcohol derives necessarily from crotonaldehyde formed by Meerwein-Ponndorf-Verley-Oppenhauer (MPVO) reduction reaction with ethanol as the reductant agent.…”

Section: Catalytic Reactionmentioning

confidence: 99%

Ca‐based bifunctional acid‐basic model‐catalysts for n‐butanol production from ethanol condensation

Pinzón

Cortés‐Reyes

Herrera

et al. 2020

Biofuels Bioprod Bioref

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Ethanol to n‐butanol conversion is a process that can increase the carbon number of alcohols by coupling. There is increasing interest in the mechanisms for n‐butanol production in a simple step through the effective use of bifunctional acid–base catalysts. In this context, commercial hydroxyapatite (HAP) and two synthetized model supported catalysts, Ca/Al2O3 and Ca‐P/Al2O3, were used in bioethanol condensation. Characterization and acid–base sites were considered, and Fourier‐transform infrared (FTIR) spectroscopy and diffuse reflectance infrared Fourier‐transform spectroscopy–mass spectrometry (DRIFT‐MS) reactivity tests were performed in situ, as a first approximation to design a sustainable catalytic process rationally, and with the aim of understanding the process at the catalytic surface. The results indicated that the reactions occur at a large range of temperatures (200–450 °C). Hydroxyapatite and Ca/Al2O3 have similar basic sites (low and medium) and Ca‐P/Al2O3 presented the strongest Brönsted and Lewis combined acid sites. Three major reactions were identified: non‐oxidative dehydrogenation, aldol condensation, and intermolecular reduction, associated with the basic‐acid sites Ca‐O‐Ca/Ca‐O‐P/Ca‐O‐Al. Side reactions also occur involving different acid sites related to Lewis alumina centers favoring ethylene or diethyl‐ether production. © 2020 Society of Industrial Chemistry and John Wiley & Sons Ltd

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“…Since 2017, the bioethanol to butanol process has been studied extensively [10][11][12][13][14][15] on a variety of catalysts. Most of those studies were conducted with anhydrous ethanol.…”

Section: Introductionmentioning

confidence: 99%

“…Most of those studies were conducted with anhydrous ethanol. Although a study [11] was carried out with hydrous ethanol (6 wt% water) in the presence of Mg-Al-oxide catalyst, the runs were very short (4 h) so no deactivation measurements were conducted. Therefore, none of those studies have tackled the important issue of water inhibition and deactivation of catalysts.…”

Section: Introductionmentioning

confidence: 99%

Eco-Friendly and Sustainable Process for Converting Hydrous Bioethanol to Butanol

et al. 2021

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The purpose of the study was the development of water-resistant catalyst and catalytic processes for the conversion of hydrous ethanol to 1-butanol. Water, in hydrous ethanol, strongly inhibits conversion to 1-butanol on solid catalysts. In this study, the nonstoichiometric P-deficient hydroxyapatite containing carbonate anions (C-HAP), Ca10−x/2(PO4)6−x(CO3)x(OH)2, displayed good performance in the Guerbet condensation of hydrated ethanol to 1-butanol, after proper stabilization of reaction conditions. Hydrous ethanol (96 wt%) was converted on C-HAP formed as extrudates with silica binder at 400 °C and weight jour space velocity (WHSV) = 0.5–1.0 h−1 to yield 21–23% 1-butanol and 73–74% selectivity. It displayed stable operation for up to 170 h on streams conducted in bench and mini-pilot rigs with catalyst loadings of 2 and 50 cm3, respectively. The process simulation employed the recycling of ethanol without laboratory verification to reach 68% theoretical yield of 1-butanol. The techno-economic analysis demonstrated the feasibility of this process, showing that it may be profitable depending on the prices of hydrated ethanol and 1-butanol.

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Successive vapour phase Guerbet condensation of ethanol and 1-butanol over Mg-Al oxide catalysts in a flow reactor

Cited by 43 publications

References 43 publications

Effect of Ni, La, and Ce Oxides on a Cu/Al₂O₃ Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

Effect of Ni, La, and Ce Oxides on a Cu/Al₂O₃ Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

Ca‐based bifunctional acid‐basic model‐catalysts for n‐butanol production from ethanol condensation

Eco-Friendly and Sustainable Process for Converting Hydrous Bioethanol to Butanol

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Successive vapour phase Guerbet condensation of ethanol and 1-butanol over Mg-Al oxide catalysts in a flow reactor

Cited by 43 publications

References 43 publications

Effect of Ni, La, and Ce Oxides on a Cu/Al2O3 Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

Effect of Ni, La, and Ce Oxides on a Cu/Al2O3 Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

Ca‐based bifunctional acid‐basic model‐catalysts for n‐butanol production from ethanol condensation

Eco-Friendly and Sustainable Process for Converting Hydrous Bioethanol to Butanol

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Effect of Ni, La, and Ce Oxides on a Cu/Al₂O₃ Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation

Effect of Ni, La, and Ce Oxides on a Cu/Al₂O₃ Catalyst with Low Copper Loading for Ethanol Non‐oxidative Dehydrogenation