State Key Laboratory Breeding Base of Photocatalysis, College of Chemistry and Chemical Engineering, Fuzhou University, Fuzhou, 350002, PR China.
ACS Appl Mater Interfaces. 2013 Feb;5(3):1156-64. doi: 10.1021/am3029798. Epub 2013 Jan 29.
A series of TiO(2)-graphene (GR), -carbon nanotube (CNT), and -fullerene (C(60)) nanocomposite photocatalysts with different weight addition ratios of carbon contents are synthesized via a combination of sol-gel and hydrothermal methods. Their structures and properties are determined by the X-ray diffraction (XRD), UV-vis diffuse reflectance spectra (DRS), transmission electron microscopy (TEM), nitrogen adsorption-desorption, and photoelectrochemical measurements. Photocatalytic selective oxidation of benzyl alcohol to benzaldehyde is employed as a model reaction to evaluate the photocatalytic activity of the TiO(2)-carbon (GR, CNT, and C(60)) nanocomposites under visible light irradiation. The results reveal that incorporating TiO(2) with carbon materials can extend the adsorption edge of all the TiO(2)-carbon nanocomposites to the visible light region. For TiO(2)-GR, TiO(2)-CNT, and TiO(2)-C(60) nanocomposites, the photocatalytic activities of the composites with optimum ratios, TiO(2)-0.1% GR, TiO(2)-0.5% CNT, and TiO(2)-1.0% C(60), are very close to each other along with the irradiation time. Furthermore, the underlying reaction mechanism for the photocatalytic selective oxidation of benzyl alcohol to benzaldehyde over TiO(2)-carbon nanocomposites has been explored using different radical scavenger techniques, suggesting that TiO(2)-carbon photocatalysts follow the analogous oxidation mechanism toward selective oxidation of benzyl alcohol. The addition of different carbon materials has no significant influence on the crystal phase, particle size, and the morphology of TiO(2). Therefore, it can be concluded, at least for nanocomposites of TiO(2)-carbon (GR, CNT, and C(60)) obtained by the present approach, that there is no much difference in essence on affecting the photocatalytic performance of semiconductor TiO(2) among these three different carbon allotropes, GR, CNT, and C(60). Our findings point to the importance of a comparative study of semiconductor-carbon photocatalysts on drawing a relatively objective conclusion rather than separately emphasizing the unique role of GR and joining the graphene gold rush.
通过溶胶-凝胶和水热法相结合,合成了一系列具有不同碳含量重量添加比的 TiO(2)-石墨烯(GR)、-碳纳米管(CNT)和 -富勒烯(C(60))纳米复合材料。通过 X 射线衍射(XRD)、紫外-可见漫反射光谱(DRS)、透射电子显微镜(TEM)、氮气吸附-脱附以及光电化学测量来确定其结构和性能。采用苯甲醇的选择性氧化作为模型反应,来评估 TiO(2)-碳(GR、CNT 和 C(60))纳米复合材料在可见光照射下的光催化活性。结果表明,将 TiO(2)与碳材料结合可以将所有 TiO(2)-碳纳米复合材料的吸收边缘扩展到可见光区域。对于 TiO(2)-GR、TiO(2)-CNT 和 TiO(2)-C(60)纳米复合材料,在最佳比例下,TiO(2)-0.1%GR、TiO(2)-0.5%CNT 和 TiO(2)-1.0%C(60)的复合材料的光催化活性非常接近,并且随着照射时间的增加而增加。此外,通过使用不同的自由基清除剂技术,探索了 TiO(2)-碳纳米复合材料光催化选择性氧化苯甲醇制苯甲醛的反应机理,表明 TiO(2)-碳光催化剂遵循类似的氧化机制,用于选择性氧化苯甲醇。不同碳材料的添加对 TiO(2)的晶体相、粒径和形貌没有显著影响。因此,可以得出结论,至少对于通过本方法获得的 TiO(2)-碳(GR、CNT 和 C(60))纳米复合材料而言,在这三种不同的碳同素异形体 GR、CNT 和 C(60)中,对半导体 TiO(2)的光催化性能的影响本质上没有太大差异。我们的研究结果表明,对于半导体-碳光催化剂进行比较研究对于得出相对客观的结论非常重要,而不是分别强调 GR 的独特作用并加入石墨烯热潮。