Calcium Phosphate Catalysts for Ethanol Coupling to Butanol and Butadiene

Prillaman, J. Tyler; Miyake, Naomi; Davis, Robert J.

doi:10.1007/s10562-020-03342-5

Cited by 5 publications

(6 citation statements)

References 38 publications

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“…The most widely accepted reaction mechanism for the Lebedev reaction is composed of cascading steps depicted in Scheme a, facilitated by a multifunctional catalyst . Initially, ethanol is dehydrogenated to form acetaldehyde.…”

Section: Introductionmentioning

confidence: 99%

“…More recently, Jones et al found that a mixture of Cu, Zn, and ZrO 2 supported on SiO 2 used in the Lebedev reaction had a relatively high selectivity of 67% toward butadiene, but the conversion was less than 50% . Prillaman et al observed an increase in selectivity toward butadiene when ZrO 2 was added to their calcium phosphate catalyst in the Lebedev reaction . Several groups have also observed an increase in butadiene yield over their MgO and SiO 2 catalyst with the addition of transition metals such as Ag and Cu. − Petrolini et al showed that the addition of Cu to their AlMgO catalyst increased selectivity toward acetaldehyde while slowing the formation of diethyl ether .…”

Section: Introductionmentioning

confidence: 99%

“…The most widely accepted reaction mechanism for the Lebedev reaction is composed of cascading steps depicted in Scheme 2a, facilitated by a multifunctional catalyst. 11 Initially, ethanol is dehydrogenated to form acetaldehyde. The acetaldehyde undergoes self-aldol condensation to crotonaldehyde, followed by hydrogenation to crotyl alcohol.…”

Section: ■ Introductionmentioning

confidence: 99%

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Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO₂ Catalysts

Miyake

Brezicki

Davis

2022

ACS Sustainable Chem. Eng.

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Although butadiene is currently a byproduct of naphtha cracking, interest in producing butadiene from biobased ethanol has increased because of the lower environmental impact of the ethanol to butadiene reaction. This work explores a multifunctional catalyst system composed of silica-supported Ag and ZrO2 used for the cascade reaction of ethanol to butadiene at 573 K. The Ag and ZrO2 components were synthesized on separate support particles, enabling the characterization of each component without interference from the other. High selectivity to butadiene (65%) at high ethanol conversion (75%) was achieved with an appropriate ratio of Ag and ZrO2 in the reactor. Silver catalyzed the initial dehydrogenation of ethanol to acetaldehyde, while ZrO2 catalyzed the C–C coupling and subsequent dehydration reactions. The silica-supported ZrO2 exhibited superior selectivity relative to bulk ZrO2 in the Ag-promoted ethanol to butadiene reaction. Results from Zr K-edge X-ray absorption spectroscopy and UV–vis spectroscopy showed that ZrO2 was highly dispersed on the silica support over a range of loadings. Infrared spectroscopy of adsorbed pyridine, CO, and CO2, and kinetics of probe reactions 1-butene double bond isomerization, 2-propanol decomposition, and ethanol hydrogenation of acetone were used to compare the acid–base nature and chemical reactivity of silica-supported ZrO2 to bulk ZrO2.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

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Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO₂ Catalysts

Miyake

Brezicki

Davis

2022

ACS Sustainable Chem. Eng.

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“…Compared to bioethanol, long-chain alcohols offer high value as fine chemicals for plasticizers, surfactants, and pharmaceutical intermediates, 7 and due to their longer carbon chains, they contribute to higher cetane numbers, higher energy densities, nonhygroscopicity, better mixing stability, and compressed ignition qualities. 8,9 Therefore, these advantages of long-chain alcohols make it of great significance to upgrade ethanol to long-chain alcohols. 10 Guerbet coupling is a promising method for the preparation of long-chain alcohols, the key steps of which include alcohol acetal and hydrogen transfer.…”

Section: Introductionmentioning

confidence: 99%

Upgrading of Aqueous Ethanol to Long-Chain Alcohols over Immobilized Highly Dispersed Ni–Re Catalyst

Zhang,

Liu,

Jiang

et al. 2024

Ind. Eng. Chem. Res.

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Motivated by the carbon neutrality policy and the demand for value-added bio-based chemicals, it is of great significance and interest to directly upgrade aqueous ethanol to produce long-chain alcohol chemicals and transportation biofuel. In this study, a bimetallic catalyst composed of Re doped Ni@C was prepared by a facile sol–gel method. The bimetal 70-NiRe@C demonstrated higher selectivity toward target long-chain alcohols product and lower selectivity of C1 byproducts than the monomeric metal Ni@C. The addition of Re promotes the dispersion of active Ni on the graphite carrier, contributing to the superior 59.9% ethanol conversion and 45.0% long-chain alcohol yield. This work guides future research into the direct upgrading of water-based bioethanol to the value-added long-chain fine chemicals and biofuels required.

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“…Also, treating Zr with oxalic acid gives well-coordinated acidic and basic surroundings if necessary. ZrO 2 , Zr/Si, and CaO/Zr-containing catalysts are usually used at a temperature of 300-425 • C, at standard pressure [10][11][12][13]. It was suggested that the catalyst activity could be correlated with the number of strong Brønsted acid sites in the catalyst.…”

Section: Introductionmentioning

confidence: 99%

Production of 1,3-Butadiene from Ethanol Using Treated Zr-Based Catalyst

Bojang¹,

Wu²

2022

Catalysts

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The conversion of ethanol to 1,3-butadiene was carried out using a treated Zr-based catalyst at a temperature of 350–400 °C with different weight hourly space velocities in a fixed bed reactor. The catalysts used are commercial, but they underwent pretreatment. The commercial catalysts used were ZrO2, Zr(OH)2, 2% CaO-ZrO2, 30% TiO2-ZrO2, 50% CeO2-ZrO2 and 10% SiO2-ZrO2 in their modified or treated form. The characterizations of the catalysts were carried out using XRD, XPS, and TGA. The results indicated that ethanol conversion, yield, and selectivity of 1,3-butadiene operated weight hourly space velocity of 2.5 h−1 using 10% SiO2-ZrO2 were 95%, 80%, and 85%, respectively, at 350 °C. Using 50% CeO2-ZrO2 converted 70% ethanol with a 1,3-butadiene yield of 65%. The best Zr-based catalyst was 10% SiO2-ZrO2 as it gives a steady 1,3-butadiene yield, the Si-composition with ZrO2 gives a good catalytic pour of the catalyst-bed structure; hence, the life span was good. Using 30% TiO2-ZrO2 has an ethanol conversion of 70% with a 1,3-butadiene yield of 43%.

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Calcium Phosphate Catalysts for Ethanol Coupling to Butanol and Butadiene

Cited by 5 publications

References 38 publications

Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO₂ Catalysts

Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO₂ Catalysts

Upgrading of Aqueous Ethanol to Long-Chain Alcohols over Immobilized Highly Dispersed Ni–Re Catalyst

Production of 1,3-Butadiene from Ethanol Using Treated Zr-Based Catalyst

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Calcium Phosphate Catalysts for Ethanol Coupling to Butanol and Butadiene

Cited by 5 publications

References 38 publications

Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO2 Catalysts

Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO2 Catalysts

Upgrading of Aqueous Ethanol to Long-Chain Alcohols over Immobilized Highly Dispersed Ni–Re Catalyst

Production of 1,3-Butadiene from Ethanol Using Treated Zr-Based Catalyst

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Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO₂ Catalysts

Cascade Reaction of Ethanol to Butadiene over Multifunctional Silica-Supported Ag and ZrO₂ Catalysts