Enhanced photocatalytic hydrogen production by improving the Pt dispersion over mesostructured TiO_2

摘要

Among other potential applications, mesoporous titania with high surface area and crystalline framework is attractive in photocatalytic hydrogen production. The mesoporous structure with pore walls formed by nanocrystals of anatase would provide a shorter distance of the electron-hole pairs to reach the photocatalyst surface and a higher surface area to deposit modifiers of its photocatalytic activity. In this work, we have successfully applied a hard-templating pathway to obtain ordered mesoporous titania (m-TiO_2) with high surface area and anatase as main crystalline phase. Subsequently, various amounts of metallic Pt have been deposited using different impregnation methods. All reactions performed exhibit, at short times, a rapid increase in the hydrogen production rate until a point in which a nearly constant value is achieved. The material prepared by the "citrate method", based on reduction and encapsulation with sodium citrate of Pt nanoparticles before the photocatalytic reaction, leads to the highest hydrogen production rates with the shortest time to reach the change on the trend of the activity curve. The reason of this result is that citrate method provides very good dispersion and, specially, because the Pt nanoparticles are deposited and reduced preferentially within the pores of m-TiO_2, leading to stronger interactions than the other two explored dispersion routes (wetness impregnation and photodeposition). Thus, despite introducing less than half of the theoretical amount of Pt, citrate method produces close to twice the amount of hydrogen obtained by the other dispersion routes. This production capacity is even higher when the amount of Pt loaded is increased, with the optimal concentration being determined as 2% (w/w).