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CATALYSIS SCIENCE & TECHNOLOGY
卷 -, 期 -, 页码 -出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d3cy01224g
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A variety of methods were used to synthesize amorphous silica-alumina (ASA) and investigate the role of aluminum species and surface area in catalytic reactions. The study found that Bronsted acidity is crucial for p-xylene formation.
A variety of methods are employed to synthesize amorphous silica-alumina (ASA) to resolve the role of Al speciation and surface area in the catalytic performance in the Diels-Alder cycloaddition reaction of 2,5-dimethylfuran and ethylene to p-xylene. ASA was prepared by homogeneous deposition-precipitation (HDP) of Al3+ on ordered mesoporous silica, i.e., SBA-15 and OMS prepared under hydrothermal synthesis conditions using an imidazole-based template, and one-step flame spray pyrolysis (FSP). IR spectroscopy and 27Al MAS NMR showed that the resulting ASA represented a set of materials with distinct textural and acidic properties. ASA prepared by grafting Al to ordered mesoporous silica led to a much higher concentration of Bronsted acid sites (BAS). These samples performed much better in the DAC reaction, with p-xylene yields higher than those obtained with a HBeta zeolite benchmark. Materials with Al partially in the bulk of silica (OMS, FSP) and containing significant alumina domains are less acidic and exhibit much lower p-xylene yields. These findings point to the importance of Bronsted acidity for p-xylene formation. This study shows that careful design of the Al speciation can lead to amorphous silica-alumina with similar DAC performance to microporous zeolites. A variety of methods are employed to synthesize amorphous silica-alumina (ASA) to resolve the role of Al speciation and surface area in the catalytic performance in the Diels-Alder cycloaddition reaction of 2,5-dimethylfuran and ethylene to p-xylene.
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