Catalytic properties of reduced graphene oxide in acetylene hydrogenation

Abakumov, Alexander; Bychko, Igor; Selyshchev, Oleksandr; Zahn, Dietrich R. T.; Qi, Xiaohua; Tang, Jianguo; Strizhak, P. E.

doi:10.1016/j.carbon.2019.10.058

Cited by 16 publications

(13 citation statements)

References 64 publications

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“…Integrated with technology of acetylene production from natural gas or coal, selective hydrogenation of acetylene to ethylene (HAE) has emerged as a promising non-oil route for producing ethylene, which is one of the most important building blocks in chemical synthesis 1 – 3 . Thermocatalytic HAE typically requires high temperatures above 200 °C and high pressures of around 5 bar 4 – 8 , and thus is highly energy demanding. Besides, large amount of H 2 consumption makes the process even more costly.…”

Section: Introductionmentioning

confidence: 99%

Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions

Wang

Uwakwe

et al. 2021

Nat Commun

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Renewable energy-based electrocatalytic hydrogenation of acetylene to ethylene (E-HAE) under mild conditions is an attractive substitution to the conventional energy-intensive industrial process, but is challenging due to its low Faradaic efficiency caused by competitive hydrogen evolution reaction. Herein, we report a highly efficient and selective E-HAE process at room temperature and ambient pressure over the Cu catalyst. A high Faradaic efficiency of 83.2% for ethylene with a current density of 29 mA cm−2 is reached at −0.6 V vs. the reversible hydrogen electrode. In-situ spectroscopic characterizations combined with first-principles calculations reveal that electron transfer from the Cu surface to adsorbed acetylene induces preferential adsorption and hydrogenation of the acetylene over hydrogen formation, thus enabling a highly selective E-HAE process through the electron-coupled proton transfer mechanism. This work presents a feasible route for high-efficiency ethylene production from E-HAE.

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Section: Introductionmentioning

confidence: 99%

Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions

Wang

Uwakwe

et al. 2021

Nat Commun

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“…Основним продуктом гідрування ацетилену є етилен, який в подальшому частково гідрується до етану. Отже, матеріали на основі ВОГ є перспективними каталізаторами для селективного гідрування С≡С-зв'язку [29].…”

Section: каталітичні властивості нановуглецевих матеріалів у реакції селективного гідрування ацетиленуunclassified

Catalytic properties of nanocarbon materials in reaction of selective hydrogenation of acetylene

Bychko¹,

Abakumov²,

Trypolskyi³

et al. 2021

New Functional Substances and Materials for Chemical Engineering

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The chapter presents the results of studies of the catalytic properties of nanocarbon materials based on carbon nanotubes and reduced graphene oxide in the hydrogenation of ethylene, acetylene and ethylene-acetylene mixture by molecular hydrogen at atmosphere pressure. The current state of scientific approaches to the creation of nanocarbon metal-free catalysts for the hydrogenation reactions in both liquid and gas phases is presented. A possible nature of active center of the hydrogenation reaction located on the surface of the nanocarbon material is discussed. It is shown that the catalytic activity of the nanocarbon materials is not associated with metal impurities. The correlation between the structural characteristics of carbon nanomaterials and their catalytic properties in the hydrogenation reactions of unsaturated hydrocarbons is demonstrated. A comparative analysis of the catalytic activity of nanocarbon materials and catalysts that contain noble metals in the hydrogenation reaction of acetylene is presented. Finally, the fundamental possibility of creating a nanocarbon catalyst for selective hydrogenation of acetylene in excess ethylene is shown.

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“…The carbocatalysts are gaining interest with the emergence of such a new class of graphene derivatives. It was demonstrated that these novel materials are applicable to a variety of reactions, such as hydrogenation, − which often requires the presence of an expensive noble metal.…”

Section: Introductionmentioning

confidence: 99%

Active Sites and Their Individual Turnover Frequencies for Ethylene Hydrogenation on Reduced Graphene Aerogel

Yalcin,

Kurtoğlu-Öztulum,

Sarac Oztuna

et al. 2024

Langmuir

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Graphene aerogel (GA) was reduced at various temperatures to prepare a series of reduced graphene aerogels (rGAs) with different surface characteristics. Detailed characterization demonstrated that an increase in the thermal reduction temperature leads to an increase in surface area accompanied by an increase in surface density of defect sites formed by the removal of the oxygencontaining functional groups. rGA samples were then tested for ethylene hydrogenation under identical conditions. A comparison of catalytic performances of each catalyst demonstrated that the rGA sample prepared by reduction in Ar at 900 °C (rGA-900) provides the highest performance compared with others prepared at lower temperatures. Next, we analyzed the per-gram activity of each catalyst as a sum of individual contributions from different defect sites quantified by Raman spectroscopy and CHNS-O analysis to determine the individual turnover frequencies (TOFs) of each active site. This analysis identified polyene-like structures and interstitial defects associated with amorphous sp 2 bonded carbon atoms as the dominant active sites responsible for hydrogenation. A comparison of their TOFs further indicated that the polyene-like structures provide approximately ten times higher TOF compared to those associated with the amorphous carbon defects. These results, identifying the dominant active centers and quantifying their corresponding TOFs, provide opportunities toward the rational design of GA-based carbocatalysts.

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Catalytic properties of reduced graphene oxide in acetylene hydrogenation

Cited by 16 publications

References 64 publications

Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions

Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions

Catalytic properties of nanocarbon materials in reaction of selective hydrogenation of acetylene

Active Sites and Their Individual Turnover Frequencies for Ethylene Hydrogenation on Reduced Graphene Aerogel

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