期刊
CHEMICAL ENGINEERING JOURNAL
卷 452, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.139303
关键词
Acetalization; Modification; Zeolite
A dual designing strategy involving Fe3+ modified Bronsted acidity and chlor-otrimethylsilane (CTS) altered hydrophilicity was proposed and validated for enhanced activity and stability of NaY catalysts in solketal synthesis from bio-oxygenates. Fe3+ exchanged NaYs showed a shortened Si-OH bond and electronically reconfigured Fe3+ sites, resulting in a 4-fold activity enhancement. Furthermore, CTS modified FeY materials improved the acetali-zation of glycerol by 18-fold and displayed remarkable stability against impurity molecules.
Solketal is known as a promising non-BPA plasticizer. However, fast and robust synthesis of solketal from bio-oxygenates remains a grand challenge, as strong surface polarization often deactivates acidic catalysts. We proposed and validated a dual designing strategy, involving (1) Fe3+ modified Bronsted acidity and (2) chlor-otrimethylsilane (CTS) altered hydrophilicity for enhanced activity and stability of NaY catalysts. As one of the key findings, Fe3+ exchanged NaYs display an unusual shortened Si-OH bond and electronically reconfigured Fe3+ sites for a 4-fold activity enhancement. Furthermore, CTS modified FeY materials further alleviate surface passivation of glycerol and water, leading to an 18-fold activity improvement and better durability for acetali-zation of glycerol. CTS modified FeY catalysts display remarkable stability against varies impurity molecules. The dual modification methodology provides useful information on rational design of durable catalysts for synthesis of various other non-BPA derivatives.
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