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Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway

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 H(2)O(2) 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...

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Autores principales: Sobczak, Izabela, Kowalska, Tsering Chödon, Nowicka, Magdalena, Ziolek, Maria
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9102529/
https://www.ncbi.nlm.nih.gov/pubmed/35563036
http://dx.doi.org/10.3390/ijms23094639
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author Sobczak, Izabela
Kowalska, Tsering Chödon
Nowicka, Magdalena
Ziolek, Maria
author_facet Sobczak, Izabela
Kowalska, Tsering Chödon
Nowicka, Magdalena
Ziolek, Maria
author_sort Sobczak, Izabela
collection PubMed
description 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 H(2)O(2) 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, N(2) 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 (E(F)), 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 H(2)O(2) adsorption, and thus, were not directly involved in the reaction pathway. Both reagents were adsorbed on gold nanoparticles. H(2)O(2) 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 E(F) has to be reached (for 5.7 nm Au NPs).
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spelling pubmed-91025292022-05-14 Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway Sobczak, Izabela Kowalska, Tsering Chödon Nowicka, Magdalena Ziolek, Maria Int J Mol Sci Article 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 H(2)O(2) 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, N(2) 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 (E(F)), 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 H(2)O(2) adsorption, and thus, were not directly involved in the reaction pathway. Both reagents were adsorbed on gold nanoparticles. H(2)O(2) 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 E(F) has to be reached (for 5.7 nm Au NPs). MDPI 2022-04-22 /pmc/articles/PMC9102529/ /pubmed/35563036 http://dx.doi.org/10.3390/ijms23094639 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Sobczak, Izabela
Kowalska, Tsering Chödon
Nowicka, Magdalena
Ziolek, Maria
Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
title Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
title_full Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
title_fullStr Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
title_full_unstemmed Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
title_short Microwave-Assisted Base-Free Oxidation of Glucose with H(2)O(2) on Gold- and Manganese-Containing SBA-15—Insight into Factors Affecting the Reaction Pathway
title_sort microwave-assisted base-free oxidation of glucose with h(2)o(2) on gold- and manganese-containing sba-15—insight into factors affecting the reaction pathway
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9102529/
https://www.ncbi.nlm.nih.gov/pubmed/35563036
http://dx.doi.org/10.3390/ijms23094639
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