Journal
MATERIALS
Volume 14, Issue 18, Pages -Publisher
MDPI
DOI: 10.3390/ma14185250
Keywords
gold zeolites; amino-organosilane modifier; boron modifier; selective glucose oxidation with O-2 and H2O2; microwave-assisted oxidation; base-free oxidation
Categories
Funding
- National Science Centre in Poland [2018/29/B/ST5/00137]
- Polish Ministry of Education and Science (Diamentowy Grant program) [DI2018 002248]
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The activity of gold supported catalysts is highly dependent on the type and composition of the support, which determines the size of Au nanoparticles and influences gold's properties. This study used two types of zeolites as supports for gold, aiming to modify their properties for different performances in the oxidation of glucose to gluconic acid. Modifications of the zeolites affected the glucose conversion rate while maintaining high selectivity.
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.
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