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Keywords = microwave-assisted glucose oxidation with H2O2

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21 pages, 2240 KiB  
Article
Microwave-Assisted Base-Free Oxidation of Glucose with H2O2 on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
by Izabela Sobczak, Tsering Chödon Kowalska, Magdalena Nowicka and Maria Ziolek
Int. J. Mol. Sci. 2022, 23(9), 4639; https://doi.org/10.3390/ijms23094639 - 22 Apr 2022
Cited by 3 | Viewed by 2422
Abstract
The aim of this work was to gain insights into the role of manganese in MnSBA-15 support for gold in the base-free glucose oxidation with H2O2 using a microwave reactor. MnSBA-15 (manganese—acidity source) and SBA-15 (for comparison) were modified with [...] Read more.
The aim of this work was to gain insights into the role of manganese in MnSBA-15 support for gold in the base-free glucose oxidation with H2O2 using a microwave reactor. MnSBA-15 (manganese—acidity source) and SBA-15 (for comparison) were modified with Au (2.2 wt. %) and Cu (for comparison). The physicochemical properties of the catalysts were investigated by XRD, N2 ads/des, TEM, UV-vis, XPS, pyridine adsorption combined with FTIR, ATR-FTIR, and 2-propanol decomposition. The effects of the Mn presence in the support, Au NPs size that determines the number of active Au centers, and the Fermi energy (EF), together with the effects of the pore size, reaction temperature, and time on the activity and selectivity of the applied catalysts were assessed and discussed. It has been demonstrated that the presence of Mn generated Lewis acid centers which did not participate in glucose and H2O2 adsorption, and thus, were not directly involved in the reaction pathway. Both reagents were adsorbed on gold nanoparticles. H2O2 was decomposed to molecular oxygen which oxidized glucose to gluconic acid (50–90% of glucose conversion depending on the reaction time and ~100% selectivity). The presence of manganese in MnSBA-15 was responsible for increased Au NPs size and only slightly influenced the negative charge on gold particles. To achieve effective activity a compromise between the number of active gold species and the level of EF has to be reached (for 5.7 nm Au NPs). Full article
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21 pages, 3743 KiB  
Article
Modification of Gold Zeolitic Supports for Catalytic Oxidation of Glucose to Gluconic Acid
by Adrian Walkowiak, Joanna Wolska, Anna Wojtaszek-Gurdak, Izabela Sobczak, Lukasz Wolski and Maria Ziolek
Materials 2021, 14(18), 5250; https://doi.org/10.3390/ma14185250 - 13 Sep 2021
Cited by 9 | Viewed by 3123
Abstract
Activity of gold supported catalysts strongly depends on the type and composition of support, which determine the size of Au nanoparticles (Au NPs), gold-support interaction influencing gold properties, interaction with the reactants and, in this way, the reaction pathway. The aim of this [...] Read more.
Activity of gold supported catalysts strongly depends on the type and composition of support, which determine the size of Au nanoparticles (Au NPs), gold-support interaction influencing gold properties, interaction with the reactants and, in this way, the reaction pathway. The aim of this study was to use two types of zeolites: the three dimensional HBeta and the layered two-dimensional MCM-36 as supports for gold, and modification of their properties towards the achievement of different properties in oxidation of glucose to gluconic acid with molecular oxygen and hydrogen peroxide. Such an approach allowed establishment of relationships between the activity of gold catalysts and different parameters such as Au NPs size, electronic properties of gold, structure and acidity of the supports. The zeolites were modified with (3-aminopropyl)-trimethoxysilane (APMS), which affected the support features and Au NPs properties. Moreover, the modification of the zeolite lattice with boron was applied to change the strength of the zeolite acidity. All modifications resulted in changes in glucose conversion, while maintaining high selectivity to gluconic acid. The most important findings include the differences in the reaction steps limiting the reaction rate depending on the nature of the oxidant applied (oxygen vs. H2O2), the important role of porosity of the zeolite supports, and accumulation of negative charge on Au NPs in catalytic oxidation of glucose. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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