Switching off H2O2 Decomposition during TS-1 Catalysed Epoxidation via Post-Synthetic Active Site Modification

Catalysts

Ceri Hammond¹  Giulia Tarantino² 

[1]Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK

[2] E-Mail

关键词: zeolites;    Lewis acid;    TS-1;    H₂O₂;    sustainable chemistry;    epoxidation;    catalysis;   

DOI  :  10.3390/catal5042309

来源: mdpi

【 摘 要 】

Despite its widespread use, the Lewis acidic zeolite, TS-1, still exhibits several unfavourable properties, such as excessive H₂O₂ decomposition, which decrease its overall performance. In this manuscript, we demonstrate that post-synthetic modification of TS-1 with aqueous NH₄HF₂ leads to modifications in epoxidation catalysis, which both improves the levels of epoxide selectivity obtained, and drastically minimises undesirable H₂O₂ decomposition. Through in situ spectroscopic study with UV-resonance enhanced Raman spectroscopy, we also observe a change in Ti site speciation, which occurs via the extraction of mononuclear [Ti(OSi)₄] atoms, and which may be responsible for the changes in observed activity.

【 授权许可】

CC BY   
© 2015 by the authors; licensee MDPI, Basel, Switzerland.