Effect of the SiO2 support on the catalytic performance of Ag/ZrO2/SiO2 catalysts for the single-bed production of butadiene from ethanol

Dagle, Vanessa Lebarbier; Flake, Matthew; Lemmon, Teresa; Lopez, Johnny Saavedra; Kovařík, Libor; Dagle, Robert A.

doi:10.1016/j.apcatb.2018.05.055

Cited by 82 publications

(106 citation statements)

References 31 publications

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“…Adding Ag to t ‐ZrO 2 or using a physical mixture composed of a Cu based catalyst and t ‐ZrO 2 , the selectivity to butadiene increases whereas the selectivity to ethylene decreases. They suggested that dehydrogenation is the slowest step of the butadiene synthesis, which is in line with Dagle's et al . work.…”

Section: Introductionsupporting

confidence: 76%

“…Lately, Dagle et al . have carried out a comprehensive study employing Ag, ZrO 2 and SiO 2 based catalysts.…”

Section: Introductionmentioning

confidence: 99%

“…The synthesis of butadiene from ethanol can be described as following (Scheme 1): firstly, ethanol is dehydrogenated to acetaldehyde; next, this aldehyde condenses and synthesizes acetaldol (aldol condensation); then crotonaldehyde is generated by the acetaldol dehydration; next, this C 4 aldehyde is hydrogenated by the Meerwein-Pondorf-Verley (MPV) mechanism to crotyl alcohol; finally, this alcohol is dehydrated to butadiene. [4][5][6][7][8][9][10] Most researchers working in this field accept this reaction system. [ Some very interesting and promising works have employed zirconia-based catalysts for the generation of butadiene from ethanol.…”

Section: Introductionmentioning

confidence: 99%

“…Lately, Dagle et al [9] have carried out a comprehensive study employing Ag, ZrO 2 and SiO 2 based catalysts. They reached high butadiene yields and verified that Ag is associated with the ethanol conversion whereas the butadiene selectivity depends on the Lewis acid sites on ZrO 2 and SiO 2 .…”

Section: Introductionmentioning

confidence: 99%

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The Role of the Oxygen Vacancies in the Synthesis of 1, 3‐Butadiene from Ethanol

et al. 2019

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The t‐ZrO2 doped with Zn catalyst and t‐ZrO2 as reference were employed in the butadiene synthesis from ethanol. Both catalysts were characterized by NH3‐TPD, CO2‐TPD, TPSR, the MPV model reaction, ICP, BET and EPR. Adding 0.2 wt% Zn to t‐ZrO2, the selectivity to butadiene increases three fold whereas the one to ethylene decreases. When ZrO2 is doped, the number of basic sites increases and the number of acid sites decreases. The TPSR spectra indicate that the acetaldehyde generation is the rate limiting step of the butadiene synthesis. The slowest step of the acetaldehyde generation is the H abstraction by a strong basic site. The EPR spectra show the replacement of Zr4+ by Zn2+ in the lattice of the t‐ZrO2 oxide. This phenomenon forms pairs of oxygen vacancies and coordinatively unsaturated Zr4+ ions (cus), which are strong basic sites and acid sites, respectively. Doping ZrO2 with Zn, the ethanol dehydrogenation and the butadiene synthesis are promoted not only due to the changes in the acidity and basicity of the catalyst but mainly because of the generation of oxygen vacancies and cus pairs during the reaction. These oxygen vacancies seem to behave as strong Brønsted basic sites.

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Section: Introductionsupporting

confidence: 76%

“…Lately, Dagle et al . have carried out a comprehensive study employing Ag, ZrO 2 and SiO 2 based catalysts.…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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The Role of the Oxygen Vacancies in the Synthesis of 1, 3‐Butadiene from Ethanol

et al. 2019

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“…27 Another crucial component of catalysts active in the Lebedev process is their ability to convert ethanol to acetaldehyde. 28 Several dehydrogenation promoters have been tested and their activity investigated: Ivanova et al proposed a mechanism for dehydrogenation on silica-supported metallic silver; 20,29 Dagle et al found silver particle size to be a crucial parameter; 30 Angelici et al and Taifan et al researched the activity and deactivation of copper on MgO-SiO 2 ; 14,31,32 Kyriienko et al compared the promoter effect of Ag, Zn and Cu on Ta-containing zeolites, identifying the latter as better suited for the Lebedev process. 33 Because the results of mechanistic studies differ from one promoter to another, it is likely that different mechanisms leading to acetaldehyde can take place depending on the catalytic system.…”

Section: Introductionmentioning

confidence: 99%

Properties and activity of Zn–Ta-TUD-1 in the Lebedev process

et al. 2020

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Solid‐Supported Catalysts for Organic Functional Group Transformations

et al. 2023

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Design of solid‐supported metal catalysts (SSMCs) has made an increasingly important contribution to heterogeneous catalysis in terms of fundamental understanding and technological applications. For instance, industrial use of supported catalysts for oxidation, reduction, and C−C bond formation reactions is highly prevalent. The reason behind this is that such catalysts are economical, have high thermal stability, dispersion, high exposed surface area, and above all, high reusability (up to multiple subsequent cycles). Such characteristics make supported catalysts ideal for green synthesis. However, unlike homogeneous catalysis, heterogeneous catalysis is widely applied in crude oil refining, the pharmaceutical industry, water purification, natural product synthesis, and environmental catalysis. Carbon‐carbon bond formation reactions are frequently used in the organic synthesis using SSMCs. SSMCs are attractive to synthetic chemists due to their easy recovery and excellent stability compared to unsupported metal catalysts. However, the major drawback of SSMCs is related to metal sintering at elevated temperatures caused by weak interactions between the metal and solid support in SSMCs. This review highlights major advancements in SSMCs. Three commonly reported solid supports for metal catalysts, such metal oxides, carbonaceous materials, and polymeric compounds, are discussed. Moreover, a series of thermo‐ and photocatalyzed reactions, such as hydrogenation, carbon‐carbon bond formation, oxidation reactions and multicomponent reactions and the effect of variable supports towards activity and selectivity are demonstrated.

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Effect of the SiO2 support on the catalytic performance of Ag/ZrO2/SiO2 catalysts for the single-bed production of butadiene from ethanol

Cited by 82 publications

References 31 publications

The Role of the Oxygen Vacancies in the Synthesis of 1, 3‐Butadiene from Ethanol

The Role of the Oxygen Vacancies in the Synthesis of 1, 3‐Butadiene from Ethanol

Properties and activity of Zn–Ta-TUD-1 in the Lebedev process

Solid‐Supported Catalysts for Organic Functional Group Transformations

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