Almohammadi Ghadeer, O'Modhrain Colin, Kelly Sean, Sullivan James A
UCD School of Chemistry, Belfield, Dublin 4, Ireland.
ACS Omega. 2019 Dec 30;5(1):791-798. doi: 10.1021/acsomega.9b03530. eCollection 2020 Jan 14.
Two Ti-SBA-15 catalysts are synthesized using techniques that should either deposit Ti atoms specifically at the SBA-15 surface or allow Ti-containing species to exist at both the surface and within the bulk of SBA-15. The materials have been characterized by Fourier transform infrared (FTIR), Raman and UV visible spectroscopies, transmission electron microscopy, scanning electron microscopy/energy-dispersive X-ray spectrometry microscopies, and N physisorption experiments. They have been applied in the total oxidation of phenol under catalytic wet air oxidation (CWAO) conditions and using photo- and plasma promotion. The materials retain the structure of SBA-15 following the doping in both cases and Ti incorporation is confirmed. The nature of the incorporated Ti remains unclear-with evidence for anatase TiO (from Raman and UV vis analysis) and evidence for atomically dispersed Ti from FTIR. In terms of reactivity, the presence of Ti in the in situ-prepared catalyst improves reactivity in the photopromoted reaction (increasing conversion from 28 to 60%), while both Ti catalysts improve reactivity in the CWAO reaction (by 7% over the in situ catalyst and by 25% over the grafted material). The presence of Ti has no beneficial effect on conversion in the plasma-promoted reaction. Here, however, Ti does affect the nature of the oxidized intermediates formed during the total phenol oxidation.
使用特定技术合成了两种Ti-SBA-15催化剂,这些技术要么将Ti原子特异性地沉积在SBA-15表面,要么使含Ti物种同时存在于SBA-15的表面和本体中。通过傅里叶变换红外光谱(FTIR)、拉曼光谱和紫外可见光谱、透射电子显微镜、扫描电子显微镜/能量色散X射线光谱显微镜以及N物理吸附实验对这些材料进行了表征。它们已被应用于催化湿式空气氧化(CWAO)条件下苯酚的完全氧化,并采用了光促进和等离子体促进。在两种情况下掺杂后,材料均保留了SBA-15的结构,并且证实了Ti的掺入。掺入的Ti的性质仍不清楚——拉曼光谱和紫外可见分析表明存在锐钛矿型TiO,而FTIR表明存在原子分散的Ti。在反应活性方面,原位制备的催化剂中Ti的存在提高了光促进反应的活性(转化率从28%提高到60%),而两种Ti催化剂都提高了CWAO反应的活性(比原位催化剂提高7%,比接枝材料提高25%)。Ti的存在对等离子体促进反应中的转化率没有有益影响。然而,在这里,Ti确实影响了苯酚完全氧化过程中形成的氧化中间体的性质。