Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm, Germany.
Beilstein J Nanotechnol. 2011;2:593-606. doi: 10.3762/bjnano.2.63. Epub 2011 Sep 15.
Aiming at model systems with close-to-realistic transport properties, we have prepared and studied planar Au/TiO(2) thin-film model catalysts consisting of a thin mesoporous TiO(2) film of 200-400 nm thickness with Au nanoparticles, with a mean particle size of ~2 nm diameter, homogeneously distributed therein. The systems were prepared by spin-coating of a mesoporous TiO(2) film from solutions of ethanolic titanium tetraisopropoxide and Pluronic P123 on planar Si(100) substrates, calcination at 350 °C and subsequent Au loading by a deposition-precipitation procedure, followed by a final calcination step for catalyst activation. The structural and chemical properties of these model systems were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), N(2) adsorption, inductively coupled plasma ionization spectroscopy (ICP-OES) and X-ray photoelectron spectroscopy (XPS). The catalytic properties were evaluated through the oxidation of CO as a test reaction, and reactivities were measured directly above the film with a scanning mass spectrometer. We can demonstrate that the thin-film model catalysts closely resemble dispersed Au/TiO(2) supported catalysts in their characteristic structural and catalytic properties, and hence can be considered as suitable for catalytic model studies. The linear increase of the catalytic activity with film thickness indicates that transport limitations inside the Au/TiO(2) film catalyst are negligible, i.e., below the detection limit.
针对具有接近真实传输性质的模型体系,我们制备并研究了由厚度为 200-400nm 的薄介孔 TiO2 薄膜和均匀分布在其中的~2nm 直径的 Au 纳米粒子组成的平面 Au/TiO2 薄膜模型催化剂。该体系是通过在平面 Si(100)衬底上旋涂乙醇钛四异丙醇盐和 Pluronic P123 的介孔 TiO2 溶液、在 350°C 下煅烧以及随后通过沉积-沉淀程序负载 Au 来制备的,最后通过煅烧步骤进行催化剂活化。这些模型体系的结构和化学性质通过 X 射线衍射(XRD)、透射电子显微镜(TEM)、N2 吸附、电感耦合等离子体原子发射光谱(ICP-OES)和 X 射线光电子能谱(XPS)进行了表征。通过 CO 的氧化作为测试反应来评估催化性能,并通过扫描质谱仪直接在薄膜上方测量反应活性。我们可以证明,薄膜模型催化剂在其特征结构和催化性能上与分散的 Au/TiO2 负载催化剂非常相似,因此可以被认为是适合催化模型研究的。催化活性随薄膜厚度的线性增加表明 Au/TiO2 薄膜催化剂内部的传输限制可以忽略不计,即低于检测限。