Sakamoto Takeshi, Nagao Daisuke, Noba Masahiro, Ishii Haruyuki, Konno Mikio
Department of Chemical Engineering, ‡Graduate School of Engineering, Tohoku University , 6-6-07 Aoba Aramaki-aza, Aoba-ku, Sendai 980-8579, Japan.
Langmuir. 2014 Jun 24;30(24):7244-50. doi: 10.1021/la5012499. Epub 2014 Jun 10.
Submicrometer-sized amorphous titania spheres incorporating Au nanoparticles (NPs) were prepared in a one-pot synthesis consisting of a sol-gel reaction of titanium(IV) isopropoxide in the presence of chloroauric acid and a successive reduction with sodium borohydride in a mixed solvent of ethanol/acetonitrile. The synthesis was allowed to prepare monodisperse titania spheres that homogeneously incorporated Au NPs with sizes of ca. 7 nm. The Au NP-loaded titania spheres underwent different crystallization processes, including 500 °C calcination in air, high-temperature hydrothermal treatment (HHT), and/or low-temperature hydrothermal treatment (LHT). Photocatalytic experiments were conducted with the Au NP-loaded crystalline titania spheres under irradiation of UV and visible light. A combined process of LHT at 80 °C followed by calcination at 500 °C could effectively crystallize titania spheres maintaining the dispersion state of Au NPs, which led to photocatalytic activity higher than that of commercial P25 under UV irradiation. Under visible light irradiation, the Au NP-titania spheres prepared with a crystallization process of LHT at 80 °C for 6 h showed photocatalytic activity much higher than a commercial product of visible light photocatalyst. Structure analysis of the visible light photocatalysts indicates the importance of prevention of the Au NPs aggregation in the crystallization processes for enhancement of photocatalytic activity.
通过一锅法合成制备了包含金纳米颗粒(NPs)的亚微米级非晶态二氧化钛球,该方法包括在氯金酸存在下异丙醇钛的溶胶 - 凝胶反应,以及随后在乙醇/乙腈混合溶剂中用硼氢化钠进行还原。该合成方法能够制备出均匀掺入尺寸约为7 nm金纳米颗粒的单分散二氧化钛球。负载金纳米颗粒的二氧化钛球经历了不同的结晶过程,包括在空气中500℃煅烧、高温水热处理(HHT)和/或低温水热处理(LHT)。在紫外光和可见光照射下,对负载金纳米颗粒的结晶二氧化钛球进行了光催化实验。80℃低温水热处理后再在500℃煅烧的联合过程能够有效地使二氧化钛球结晶,同时保持金纳米颗粒的分散状态,这使得在紫外光照射下其光催化活性高于商业P25。在可见光照射下,通过80℃低温水热处理6 h的结晶过程制备的金纳米颗粒 - 二氧化钛球表现出比可见光光催化剂商业产品高得多的光催化活性。可见光光催化剂的结构分析表明,在结晶过程中防止金纳米颗粒聚集对于提高光催化活性至关重要。