空心鼓状多级孔钛硅氧化物的合成及氧化-吸附脱硫性能研究

Study on synthesis and oxidative⁃adsorptive desulfurization performance of hierarchically mesoporous titanium⁃containing silica

燃料油中的含硫化合物燃烧后会形成SOx排放到空气中,不仅引起环境污染,而且危害人类健康。因此,温和条件下的超深度脱硫技术已成为众多科研工作者关注的焦点。以表面活性剂-聚电解质形成的介观复合物为模板,成功合成了空心鼓状含钛多级孔结构二氧化硅材料。通过小角X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、氮气吸附-脱附以及紫外-可见光谱表征发现,所得到的含钛二氧化硅材料具有立方Pm-3n有序介观相态、多级介孔结构和较高骨架钛含量。由于多级介孔结构和丰富骨架钛活性位点的存在,该二氧化硅在室温下表现出优良的氧化脱硫催化活性和稳定性。此外,含钛二氧化硅对强极性氧化产物砜具有明显的吸附作用,实现了氧化-吸附一步法脱硫。

The organic sulfur compounds in transportation fuel were converted to SO;during the combustion,which not only caused serious pollution of environment,but also harmed human health.So,the ultra-deep desulfurization technology of fuel oil under moderate condition has become the focus of many scientific researchers.The hollow drum-shaped titanium-containing silica with hierarchically mesoporous structure was successfully synthesized by using a polyelectrolyte-surfactant mesomorphous complex templating method.Through characterization,including small-angle X-ray diffraction(XRD),electron scanning electron microscopy(SEM),electron transmission electron microscopy(TEM),nitrogen adsorption-desorption and ultraviolet-visible spectroscopy,the obtained hierarchically porous titanium-containing silica material possessed ordered cubic Pm-3n mesomorphous phase,hierarchically mesoporous architecture,and high framework titanium content.Owing to the secondary mesoporous structure and plentiful titanium active sites in the framework,the porous silica exhibited superior catalytic oxidative desulfurization performance and cycling stability at room temperature.In addition,the titaniumcontaining silica possessed strong adsorptive effect toward the oxidative product with strong polarity,which achieved oxidative-adsorptive process for one-pot desulfurization.