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- Hydroisomerization of n-decane over SAPO-11 catalysts synthesized with methylamine as co-templatePublication . Bertolo, Raquel; Fernandes, Auguste; Ribeiro, Filipa; Silva, João; Martins, Ângela; Ribeiro, Fernando RamoaThe present work deals with preliminary studies concerning a new synthesis approach to prepare SAPO materials with AEL structure and evaluate their catalytic behavior in the hydroisomerization of long paraffins. The new SAPO-11 catalysts were synthesized with the help of a small amine (methylamine, MA) added during the preparation of the initial gel. As MA incorporates into the structure of the final materials, it contributes, together with DPA (dipropylamine), to an increase in Si incorporation as isolated species, which results in Bronsted acid sites. Thus, this new and original synthesis strategy allows to obtain materials with enhanced Bronsted acidity when compared with free MA materials. The catalysts were tested in n-decane hydroisomerization (n-decane was used as a model molecule) and confirmed the effect of MA on the acidic properties of the catalysts. The samples synthesized with MA present a higher number of acid sites that increase the catalytic conversion but have a negative effect in the isomerization selectivity, i.e. a more significant amount of cracking products is formed.
- Incorporation of niobium in SAPO-11 materials: Synthesis and characterizationPublication . Bertolo, Raquel; Martins, Angela; Silva, João; Ribeiro, Filipa; Ribeiro, Fernando Ramoa; Fernandes, AugusteThe present work concerns a new synthesis approach to prepare niobium based SAPO materials with AEL structure and the characterization ofNb species incorporated within the inorganic matrixes. The SAPO-11 materials were synthesized with or without the help of a small amine, methylamine (MA) as co-template, while Nb was added directly during the preparation of the initial gel. Structural, textural and acidic properties of the different supports were evaluated by XRD, TPR, UV-Vis spectroscopy, pyridine adsorption followed by IR spectroscopy and thermal analyses. Pure and well crystalline Nb based SAPO-11 materials were obtained, either with or without MA, using in the initial gel a low Si content of about 0.6. Increasing the Si content of the gel up to 0.9 led to an important decrease of the samples crystallinity. Niobium was found to incorporate the AEL pores support as small Nb2O5 oxide particles and also as extra framework cationic species (Nb5+), compensating the negative charges from the matrix and generating new Lewis acid sites. (C) 2011 Elsevier Inc. All rights reserved.
- Enhancement of sintering resistance of CaO-based sorbents using industrial waste resources for Calooping in the cement industryPublication . Teixeira, P.; Mohamed, Ismail; Fernandes, Auguste; Silva, João; Ribeiro, M Filipa; Pinheiro, CarlaKeeping a high stability and CO2 capture capacity of CaO-based sorbents during the Ca-looping process is still a challenge. The main goal and the innovative idea addressed in this study consists of investigating if solid industrial waste resources such as a coal fly ash (CFA) and a spent Fluid Catalytic Cracking (SFCC) catalyst, can be used as particle spacers to improve the sintering resistance of two CaO-based sorbents. These two inert industrial waste materials are used in the present work for increasing the CaO particles separation and consequently, reducing their coalescence and hindering severe sintering at the high Ca-looping temperatures. There are currently no studies in the literature on the use of industrial SFCC wastes in blends with CaO based sorbents acting as CaO particles spacer with the objective of reducing the Ca-looping sorbents deactivation along the cycles of carbonation-calcination. Despite the mineralogical and textural differences between the CFA and SFCC catalyst industrial wastes, the tests carried out in a fixed bed laboratory reactor showed that the addition of a small fraction of waste to the CaO sorbent (ca. 10%) seems to be an interesting option to improve the CO2 capture technology efficiency. During the Ca-looping, the volume and stability of sorbent mesopores is essential to achieve higher and stable carbonation conversion values, and since the CFA and SFCC increase the SBET, they contribute to enhance the sintering resistance. The innovative results presented in this study show that the industrial CFA and SFCC wastes have potential to be an economically attractive option thus contributing to reduce the cost of the Ca-looping cycle CO2 capture process, as well as to minimize the adverse environmental impacts of the high volume of industrial wastes generated.
- Effects of oxidante acid treatments on carbon-templated hierarchical SAPO-11 materials: synthesis, characterization and catalytic evaluation in n-decane hydroiosomerizationPublication . Bertolo, Raquel; Silva, João; Ribeiro, Filipea; Maldonado-Hodar, Francisco J.; Fernandes, Auguste; Martins, Ângela Maria PereiraHierarchical SAPO-11 was synthesized using a commercial Merck carbon as template. Oxidant acid treatments were performed on the carbon matrix in order to investigate its influence on the properties of SAPO-11. Structural, textural and acidic properties of the different materials were evaluated by XRD, SEM, N-2 adsorption, pyridine adsorption followed by IR spectroscopy and thermal analyses. The catalytic behavior of the materials (with 0.5 wt.% Pt, introduced by mechanic mixture with Pt/Al2O3), were studied in the hydroisomerization of n-decane. The hierarchical samples showed higher yields in monobranched isomers than typical microporous SAPO-11, as a direct consequence of the modification on both porosity and acidity, the later one being the most predominant. (C) 2014 Elsevier B.V. All rights reserved.