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

被引：22

作者：

Hammond, Ceri ^{[1
]}

Tarantino, Giulia ^{[1
]}

机构：

[1] Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Cardiff CF10 3AT, S Glam, Wales

来源：

CATALYSTS | 2015年 / 5卷 / 04期

关键词：

zeolites; Lewis acid; TS-1; H2O2; sustainable chemistry; epoxidation; catalysis; MODIFIED TITANIUM SILICALITE; HYDROGEN-PEROXIDE; SELECTIVE OXIDATION; RAMAN-SPECTROSCOPY; IN-SITU; REACTIVITY; PROPYLENE; ZEOLITE; MECHANISMS; EVOLUTION;

D O I：

10.3390/catal5042309

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

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.

引用

页码：2309 / 2323

页数：15

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