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Título: | A hydrothermally stable transition alumina by condensation-enhanced self-assembly and pyrolysis crystallization: Application in the steam reforming of methane |
Autor: | López Pérez, Lidia; Álvarez Galván, María Consuelo; Zarubina, Valeriya; Figueiredo Fernandes, Bruno O.; Melián-Cabrera, Ignacio | Fecha de publicación: | 12-jun-2014 | Editor: | Royal Society of Chemistry (UK) | Citación: | CrystEngComm 16: 6775-6783 (2014) | Resumen: | The preparation of a steam-based hydrothermally stable transition alumina is reported. The gel was derived from a synthetic sol–gel route where Al-tri-sec-butoxide is hydrolysed in the presence of a non-ionic surfactant (EO20PO70EO20), HCl as the catalyst and water (H2O/Al = 6); the condensation was enhanced by treating the hydrolysed gel with tetrabutylammonium hydroxide (TBAOH), after which it was dried at 60 °C by solvent evaporation. The so-obtained mesophase was crystallized under argon at 1200 °C (1 h) producing a transition alumina containing δ/α, and possibly θ, alumina phases. Due to its surface acidity, the pyrolysis conditions transform the block copolymer into a cross-linked char structure that embeds the alumina crystallites. Calcination at 650 °C generates a fully porous material by burning the char; a residual carbon of 0.2 wt.% was found, attributed to the formation of surface (oxy)carbides. As a result, this route produces a transition alumina formed by nanoparticles of about 30 nm in size on average, having surface areas in the range of 59–76 m2 g−1 with well-defined mesopores centered at 14 nm. The material withstands steam at 900 °C with a relative surface area rate loss lower than those reported for δ-aluminas, the state-of-the-art MSU-X γ-alumina and other pure γ-aluminas. The hydrothermal stability was confirmed under relevant CH4 steam reforming conditions after adding Ni; a much lower surface area decay and higher CH4 conversion compared to a state-of-the-art MSU-X based Ni catalyst were observed. Two effects are important in explaining the properties of such an alumina: the char protects the particles against sintering, however, the dominant effect is provided by the TBAOH treatment that makes the mesophase more resistant to coarsening and sintering. | Versión del editor: | https://doi.org/10.1039/C4CE00880D | URI: | http://hdl.handle.net/10261/186826 | DOI: | 10.1039/c4ce00880d | ISSN: | 1466-8033 |
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