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- ItemRelations between Structure, Activity and Stability in C3N4 Based Photocatalysts Used for Solar Hydrogen Production(Basel : MDPI, 2018-1-29) Sivasankaran, Ramesh P.; Rockstroh, Nils; Hollmann, Dirk; Kreyenschulte, Carsten R.; Agostini, Giovanni; Lund, Henrik; Acharjya, Amitava; Rabeah, Jabor; Bentrup, Ursula; Junge, Henrik; Thomas, Arne; Brückner, AngelikaSolar hydrogen production from water could be a sustainable and environmentally friendly alternative to fossil energy carriers, yet so far photocatalysts active and stable enough for large-scale applications are not available, calling for advanced research efforts. In this work, H2 evolution rates of up to 1968 and 5188 μmol h−1 g−1 were obtained from aqueous solutions of triethanolamine (TEOA) and oxalic acid (OA), respectively, by irradiating composites of AgIn5S8 (AIS), mesoporous C3N4 (CN, surface area >150 m2/g) and ≤2 wt.% in-situ photodeposited Pt nanoparticles (NPs) with UV-vis (≥300 nm) and pure visible light (≥420 nm). Structural properties and electron transport in these materials were analyzed by XRD, STEM-HAADF, XPS, UV-vis-DRS, ATR-IR, photoluminescence and in situ-EPR spectroscopy. Initial H2 formation rates were highest for Pt/CN, yet with TEOA this catalyst deactivated by inclusion of Pt NPs in the matrix of CN (most pronounced at λ ≥ 300 nm) while it remained active with OA, since in this case Pt NPs were enriched on the outermost surface of CN. In Pt/AIS-CN catalysts, Pt NPs were preferentially deposited on the surface of the AIS phase which prevents them from inclusion in the CN phase but reduces simultaneously the initial H2 evolution rate. This suggests that AIS hinders transport of separated electrons from the CN conduction band to Pt NPs but retains the latter accessible by protons to produce H2.
- ItemDetermining the location of Co2+ in zeolites by UV-Vis diffuse reflection spectroscopy : A critical view(Basel : MDPI, 2020) Bellmann, Andrea; Rautenberg, Christine; Bentrup, Ursula; Brückner, AngelikaUV-Vis spectroscopy as well as in situ FTIR spectroscopy of pyridine and CO adsorption were applied to determine the nature of Co species in microporous, mesoporous, and mixed oxide materials like Co-ZSM-5, Co/Na-ZSM-5, Co/Al-SBA-15, and Co/Al2O3-SiO2. Because all sample types show comparable UV-Vis spectra with a characteristic band triplet, the former described UV-Vis band deconvolution method for determination and quantification of individual cationic sites in the zeolite appears doubtful. This is also confirmed by results of pyridine and CO adsorption revealing that all Co-zeolite samples contain two types of Co2+ species located at exchange positions as well as in oxide-like clusters independent of the Co content, while in Co/Al-SBA-15 and Co/Al2O3-SiO2 only Co2+ species in oxide-like clusters occur. Consequently, the measured UV-Vis spectra represent not exclusively isolated Co2+ species, and the characteristic triplet band is not only related to γ-, β-, and α-type Co2+ sites in the zeolite but also to those dispersed on the surface of different oxide supports. The study demonstrates that for proper characterization of the formed Co species, the use of complementary methods is required. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemNb-modified Ce/Ti oxide catalyst for the selective catalytic reduction of NO with NH3 at low temperature(Basel : MDPI, 2018) Mosrati, Jawaher; Atia, Hanan; Eckelt, Reinhard; Lund, Henrik; Agostini, Giovanni; Bentrup, Ursula; Rockstroh, Nils; Keller, Sonja; Armbruster, Udo; Mhamdi, MouradRecently, great attention has been paid to Ceria-based materials for selective catalytic reduction (SCR) with NH3 owing to their unique redox, oxygen storage, and acid-base properties. Two series of bimetallic catalysts issued from Titania modified by Ce and Nb were prepared by the one-step sol-gel method (SG) and by the sol-gel route followed by impregnation (WI). The resulting core-shell and bulk catalysts were tested in NH3-SCR of NOx. The impregnated Nb5/Ce40/Ti100 (WI) catalyst displayed 95% NOx conversion at 200 °C (GHSV = 60,000 mL·g−1·h−1, 1000 ppm NOx, 1000 ppm NH3, 5% O2/He) without forming N2O. The catalysts were characterized by various methods including ICP-OES, N2-physisorption, XRD, Raman, NH3-TPD, DRIFTS, XPS, and H2-TPR. The results showed that the introduction of Nb decreases the surface area and strengthens the surface acidity. This behavior can be explained by the strong interaction between Ceria and Titania which generates Ce-O-Ti units, as well as a high concentration of amorphous or highly dispersed Niobia. This should be the reason for the excellent performance of the catalyst prepared by the sol-gel method followed by impregnation. Furthermore, Nb5/Ce40/Ti100 (WI) has the largest NH3 adsorption capacity, which is helpful to promote the NH3-SCR reaction. The long-term stability and the effect of H2O on the catalysts were also evaluated.