Synthesis and characterization of 3-[N,N′-bis-3-(salicylidenamino)ethyltriamine] Mo(VI)O2@SBA-15: a highly stable and reusable catalyst for epoxidation and sulfoxidation reactions
Synthesis and characterization of 3-[N,N′-bis-3-(salicylidenamino)ethyltriamine] Mo(VI)O2@SBA-15: a highly stable and reusable catalyst for epoxidation and sulfoxidation reactions
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3-[N,N-bis-3-(水杨基氨基)乙基三胺] Mo(VI)O2@SBA-15的合成和表征：一种高度稳定且可重复使用的环氧化和磺氧化反应催化剂
DOI：
10.1039/c3ra47222a
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发表时间：
2014
期刊：
影响因子：
3.9
通讯作者：
A. P. Singh
中科院分区：
文献类型：
--
作者：
A. Lazar;W. R. Thiel;A. P. Singh
通过将3-[N，N′-双-3-（水杨醛缩氨基）乙基三胺]（L或Salpr）锚定在有机官能化SBA-15的内表面，并与Mo（VI）O2（acac）2络合，合成了高效且可重复使用的氧化催化剂3-[N，N′-双-3-（水杨醛缩氨基）乙基三胺] Mo（VI）O2@SBA-15。通过元素分析、ICP-OES、XRD、N2吸附、TG & DTA、固体13 C、29 Si NMR、FT-IR、拉曼光谱、XPS、DRS UV-Vis光谱、SEM和TEM等手段对催化剂的物化性能进行了表征。XRD和N2吸附分析有助于找出所合成的催化剂的形态和结构特性，并确认即使在多步合成程序后仍保留有序的介孔通道结构。SBA-15中的（100）、（110）和（200）反射提供了良好的结构稳定性、长程有序和高孔壁厚度的存在的暗示。TG和DTA结果表明，（L）Mo（VI）O2@SBA-15在300 °C下仍保持热稳定性。通过固态13 C NMR和FT-IR光谱法测定了固定在SBA-15载体表面上的有机部分。此外，固态29 Si NMR光谱提供了关于表面硅烷醇基团与有机部分的官能化程度的信息。利用拉曼光谱、XPS和DRS UV-Vis技术对（L）Mo（VI）O2@SBA-15中的电子环境和钼位的氧化态进行了监测。此外，所合成的催化剂的形貌和地形信息，证实了通过SEM和TEM图像。结果表明，（L）Mo（VI）O2@SBA-15具有较高的转化率和选择性，并具有较高的稳定性。锚定的固体催化剂可以有效地回收利用，并重复使用几次，而不会有重大的活性损失。此外，还进行了谢尔顿的热过滤试验。
The efficient and reusable oxidation catalyst 3-[N,N′-bis-3-(salicylidenamino)ethyltriamine] Mo(VI)O2@SBA-15 has been synthesized by the anchoring of the 3-[N,N-bis-3-(salicylidenamino)ethyltriamine] ligand (L or Salpr) on the inner surfaces of organofunctionalized SBA-15 and subsequent complexation with Mo(VI)O2(acac)2. The physico-chemical properties of the functionalized catalysts were analyzed by elemental analysis, ICP-OES, XRD, N2-sorption measurements, TG & DTA, solid state 13C, 29Si NMR spectroscopy, FT-IR, Raman spectroscopy, XPS, DRS UV-Vis spectroscopy, SEM and TEM. XRD and N2 sorption analyses helped to find out the morphological and textural properties of the synthesized catalysts and confirm that an ordered mesoporous channel structure was retained even after the multistep synthetic procedures. The (100), (110) and (200) reflections in SBA-15 provide hints of a good structural stability, the existence of long range ordering and a high pore wall thickness. TG and DTA results reveal that the thermal stability of (L)Mo(VI)O2@SBA-15 was maintained up to 300 °C. The organic moieties anchored over the surface of the SBA-15 support were determined by solid state 13C NMR and FT-IR spectroscopy. Further, solid state 29Si NMR spectroscopy provides the information about the degree of functionalization of the surface silanol groups with the organic moiety. The electronic environment and the oxidation state of the molybdenum site in (L)Mo(VI)O2@SBA-15 were monitored by Raman spectroscopy, XPS and DRS UV-Vis techniques. Moreover, the morphology and topographic information of the synthesized catalysts were confirmed by SEM and TEM imaging. The synthesized catalysts were evaluated in epoxidation and sulfoxidation reactions, and the results show that (L)Mo(VI)O2@SBA-15 exhibits high conversion and selectivity towards epoxidation and sulfoxidation reactions in combination with high stability. The anchored solid catalysts can be recycled effectively and reused several times without major loss in activity. In addition, Sheldon's hot filtration test was also carried out.
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