Journal
FUEL
Volume 342, Issue -, Pages -Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.127004
Keywords
Anthraquinone hydrogenation; Pd catalyst; Hydrophobicity; Electron transfer
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In this study, a amine-modified catalyst, Pd/A/SiO2, was designed and synthesized for anthraquinone (AQ) hydrogenation. Multiple techniques were used to characterize the catalysts' structural and electronic properties. The results showed that Pd/A/SiO2 exhibited superior performance and selectivity in AQ hydrogenation, providing insights for the development of highly efficient catalysts.
The development of anthraquinone (AQ) hydrogenation catalysts with high activity and selectivity remains a challenge, but it is critical in industrial applications from both economic and environmental perspectives. In this work, an amine-modified catalyst, i.e., Pd/A/SiO2, was designed and synthesized via grafting 3-aminopropyltri-methoxysilane (APTMS) onto silica support and then loading Pd via the Shiff-base reaction. Multiple techniques were used to thoroughly characterize and analyze the catalysts' structural and electronic properties, such as transmission electron microscopy (TEM), H2 temperature-programmed reduction (H2-TPR), and X-ray photo-electron spectroscopy (XPS), etc. The Pd particle size (3.86 nm) in Pd/A/SiO2 was found to be very close to the reported optimal value, which balances well between the number of active sites and the required size for AQ adsorption; also, the residual carbon species from APTMS improves the hydrophobic properties of the support, which benefits AQ adsorption and anthrahydroquinone (AQH2) desorption; and furthermore, the electron transferred from N to Pd increases the electron density of the latter, favoring the activation of the C--O bond in AQ. These factors combine to give a very superior performance of Pd/A/SiO2 for AQ hydrogenation, including a hydrogenation efficiency as high as 15.7 g/L with an intriguing selectivity of 96.1 %, and a good reusability merit within a six-run test, all of which are among the best results reported so far. This work, we believe, provides food for thought in the development of a highly efficient catalyst for AQ hydrogenation.
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