Ikeue K, Yamashita H, Takewaki T, Davis M E, Anpo M
Department of Applied Chemistry, Graduate School of Engineering, Osaka Prefecture University, Sakai, Japan.
J Synchrotron Radiat. 2001 Mar 1;8(Pt 2):602-4. doi: 10.1107/s0909049500014394.
A characterization of Ti-Beta zeolites synthesized under various conditions as well as an investigation of their photocatalytic properties for the reduction of CO2 with H2O at 323 K to produce CH4 and CH3OH were carried out. In situ XAFS spectra measurements indicated that a highly dispersed tetrahedral titanium oxide species was present in the zeolite framework and an increase in the coordination number of the titanium oxide species by the addition of H2O and CO2 molecules could be detected. The Ti-Beta zeolite having a hydrophilic property (Ti-Beta(OH)) exhibited a more dramatic increase in the coordination number than the Ti-Beta(F) zeolite which had a hydrophobic property. These results suggest that CO2 and H2O molecules can be adsorbed efficiently onto the highly dispersed tetrahedrally coordinated titanium oxide species. UV irradiation of these Ti-Beta zeolite catalysts in the presence of H2O and CO2 led to the formation of CH4 and CH3OH. Ti-Beta(OH) exhibited a higher reactivity than Ti-Beta(F), while the selectivity for the formation of CH3OH on Ti-Beta(F) was higher than that for Ti-Beta(OH). These results indicated that the reactivity and selectivity of the zeolite catalyst can be determined by the hydrophilic and hydrophobic properties of the zeolites.
对在各种条件下合成的钛-β沸石进行了表征,并对其在323 K下用H2O还原CO2以生成CH4和CH3OH的光催化性能进行了研究。原位XAFS光谱测量表明,沸石骨架中存在高度分散的四面体氧化钛物种,并且可以检测到通过添加H2O和CO2分子,氧化钛物种的配位数增加。具有亲水性的钛-β沸石(Ti-Beta(OH))比具有疏水性的钛-β沸石(Ti-Beta(F))表现出更显著的配位数增加。这些结果表明,CO2和H2O分子可以有效地吸附到高度分散的四面体配位氧化钛物种上。在H2O和CO2存在下对这些钛-β沸石催化剂进行紫外线照射导致生成CH4和CH3OH。Ti-Beta(OH)表现出比Ti-Beta(F)更高的反应活性,而Ti-Beta(F)上CH3OH形成的选择性高于Ti-Beta(OH)。这些结果表明,沸石催化剂的反应活性和选择性可以由沸石的亲水性和疏水性决定。