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Morphology, Optical Properties and Photocatalytic Activity of Photo- and Plasma-Deposited Au and Au/Ag Core/Shell Nanoparticles on Titania Layers

2018-7-6, Müller, Alexander, Peglow, Sandra, Karnahl, Michael, Kruth, Angela, Junge, Henrik, Brüser, Volker, Scheu, Christina

Titania is a promising material for numerous photocatalytic reactions such as water splitting and the degradation of organic compounds (e.g., methanol, phenol). Its catalytic performance can be significantly increased by the addition of co-catalysts. In this study, Au and Au/Ag nanoparticles were deposited onto mesoporous titania thin films using photo-deposition (Au) and magnetron-sputtering (Au and Au/Ag). All samples underwent comprehensive structural characterization by grazing incidence X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). Nanoparticle distributions and nanoparticle size distributions were correlated to the deposition methods. Light absorption measurements showed features related to diffuse scattering, the band gap of titania and the local surface plasmon resonance of the noble metal nanoparticles. Further, the photocatalytic activities were measured using methanol as a hole scavenger. All nanoparticle-decorated thin films showed significant performance increases in hydrogen evolution under UV illumination compared to pure titania, with an evolution rate of up to 372 μL H2 h−1 cm−2 representing a promising approximately 12-fold increase compared to pure titania.

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Low-Temperature Steam Reforming of Natural Gas after LPG-Enrichment with MFI Membranes

2018-12-12, Seeburg, Dominik, Liu, Dongjing, Dragomirova, Radostina, Atia, Hanan, Pohl, Marga-Martina, Amani, Hadis, Georgi, Gabriele, Kreft, Stefanie, Wohlrab, Sebastian

Low-temperature hydrogen production from natural gas via steam reforming requires novel processing concepts as well as stable catalysts. A process using zeolite membranes of the type MFI (Mobile FIve) was used to enrich natural gas with liquefied petroleum gas (LPG) alkanes (in particular, propane and n-butane), in order to improve the hydrogen production from this mixture at a reduced temperature. For this purpose, a catalyst precursor based on Rh single-sites (1 mol% Rh) on alumina was transformed in situ to a Rh1/Al2O3 catalyst possessing better performance capabilities compared with commercial catalysts. A wet raw natural gas (57.6 vol% CH4) was fully reformed at 650 °C, with 1 bar absolute pressure over the Rh1/Al2O3 at a steam to carbon ratio S/C = 4, yielding 74.7% H2. However, at 350 °C only 21 vol% H2 was obtained under these conditions. The second mixture, enriched with LPG, was obtained from the raw gas after the membrane process and contained only 25.2 vol% CH4. From this second mixture, 47 vol% H2 was generated at 350 °C after steam reforming over the Rh1/Al2O3 catalyst at S/C = 4. At S/C = 1 conversion was suppressed for both gas mixtures. Single alkane reforming of C2–C4 showed different sensitivity for side reactions, e.g., methanation between 350 and 650 °C. These results contribute to ongoing research in the field of low-temperature hydrogen release from natural gas alkanes for fuel cell applications as well as for pre-reforming processes.