Promoting effect of solvent on Cu/CoO catalyst for selective glycerol oxidation under alkaline conditions

Dodekatos, Georgios; Ternieden, Jan; Schünemann, Stefan; Weidenthaler, Claudia; Tüysüz, Harun

doi:10.1039/c8cy01284a

Cited by 14 publications

(10 citation statements)

References 56 publications

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“…Such catalyst was employed to comparatively study the solvent effects on the base-free oxidation of glycerol with oxygen in aqueous or ethanol solution, and then to probe whether and to what degree water plays a crucial role in the reaction. It is noted that the absolute ethanol as the referenced solvent well mixes with glycerol and has higher oxygen solubility than the water (Dodekatos et al, 2018b), and no additional side reactions, i.e., absolute ethanol oxidation over the same Pt/CNTs catalyst under the reaction conditions, are observed according to preliminary experimental results. It can be obviously seen in Fig.…”

Section: Solvent Effects and Kinetic Isotope Effectsmentioning

confidence: 76%

Reaction mechanism and kinetics for Pt/CNTs catalyzed base-free oxidation of glycerol

Gan

Pan

et al. 2019

Chemical Engineering Science

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Fundamental understanding of heterogeneously catalyzed aerobic, base-free oxidation of glycerol is highly desirable for sustainable and highly efficient chemical synthesis. In this work, Pt/CNTs catalyzed base-free oxidation of glycerol is investigated by combining experiments, DFT calculations and kinetics analysis. The solvent effects and kinetic isotope effects measurements as well as DFT calculations reveal that water-assisted O2 activation to form active OH* intermediates is not in rate-determining step (RDS) but in equilibrium. Then, Langmuir-Hinshelwood kinetic models are developed and fitted with the experimental data. The OH*-assisted C-H bond cleavage of glycerol is discriminated as the RDS for the two parallel oxidation pathways of glycerol via primary or secondary hydroxyl groups, where the former case exhibits lower activation energy. The insights revealed here could guide the design and optimization of this catalytic process to generate the targeted products.

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Section: Solvent Effects and Kinetic Isotope Effectsmentioning

confidence: 76%

Reaction mechanism and kinetics for Pt/CNTs catalyzed base-free oxidation of glycerol

Gan

Pan

et al. 2019

Chemical Engineering Science

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“…By IR spectroscopy, it is possible to study different dioxygen species due to the characteristic stretching vibrations of adsorbed molecular oxygen, superoxide, and peroxide. [96a,113] To identify a superoxide intermediate, in situ IR spectroscopy has been used in combination with isotope labeling using 18 O 2 over a SrMnO 3 catalyst. [95k] By applying in situ ATR-IR spectroscopy, the reaction progress in cyclohexene oxidation was monitored.…”

Section: Liquid-phase Oxidationmentioning

confidence: 99%

“…A similar promotional effect has also been observed in 1‐ and 2‐octanol oxidation over Pt/C catalysts and in the oxidation of a range of primary alcohols over bimetallic AuPt and AuPd catalysts [16] . Indeed, solvent effects are known to influence reactivity over supported nanoparticulate catalysts (Figure 1‐A); they can reduce performance through competitive adsorption [17] or indeed promote performance through facilitating kinetically relevant transformations [18] …”

Section: Catalysts For Alcohol Oxidationmentioning

confidence: 99%

A Perspective on Heterogeneous Catalysts for the Selective Oxidation of Alcohols

Najafishirtari

Ortega

Douthwaite

et al. 2021

Chemistry A European J

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Selective oxidation of higher alcohols using heterogeneous catalysts is an important reaction in the synthesis of fine chemicals with added value. Though the process for primary alcohol oxidation is industrially established, there is still a lack of fundamental understanding considering the complexity of the catalysts and their dynamics under reaction conditions, especially when higher alcohols and liquid-phase reaction media are involved. Additionally, new materials should be developed offering higher activity, selectivity, and stability. This can be achieved by unraveling the structure-performance correlations of these catalysts under reaction conditions. In this regard, researchers are encouraged to develop more advanced characterization techniques to address the complex interplay between the solid surface, the dissolved reactants, and the solvent. In this mini-review, we report some of the most important approaches taken in the field and give a perspective on how to tackle the complex challenges for different approaches in alcohol oxidation while providing insight into the remaining challenges.

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“…In addition to nickel, another non-precious catalyst alternative to noble metals for the selective oxidation of alcohols is copper [112]. CuCo [113], Cu/CoO [114,115] and Cu/Al 2 O 3 [116] couples were investigated as nonprecious metal for GOR oxidation. For CuCo-based materials prepared by co-precipitation, CoO(OH) in contact with CuO was identified as the potentially active phase.…”

Section: Non-precious Metal Catalystsmentioning

confidence: 99%

Glycerol Electro-Oxidation in Alkaline Media and Alkaline Direct Glycerol Fuel Cells

Antolini¹

2019

Catalysts

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The low price, highly active triol structure, high volumetric energy density, simple storage and environment-friendly properties make glycerol a promising fuel for an alkaline direct alcohol fuel cell (ADAFC). Unlike other ADAFCs, alkaline direct glycerol fuel cells (ADGFCs) can be used either to generate only energy (the common use of fuel cells) or to produce both energy and valuable chemicals. This work presents an overview of catalysts for glycerol oxidation in alkaline media, and their use in ADGFCs. A particular attention was paid to binary and ternary catalysts able both to increase the selectivity to valuable C3 glycerol oxidation products, reducing the C-C bond cleavage, and simultaneously to enhance glycerol conversion.

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Promoting effect of solvent on Cu/CoO catalyst for selective glycerol oxidation under alkaline conditions

Abstract: Cu/CoO catalysts were employed for the selective oxidation of glycerol in the aqueous phase under basic conditions.

Cited by 14 publications

References 56 publications

Reaction mechanism and kinetics for Pt/CNTs catalyzed base-free oxidation of glycerol

Reaction mechanism and kinetics for Pt/CNTs catalyzed base-free oxidation of glycerol

A Perspective on Heterogeneous Catalysts for the Selective Oxidation of Alcohols

Glycerol Electro-Oxidation in Alkaline Media and Alkaline Direct Glycerol Fuel Cells

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