resumo
The oligomerisation of 1-butene was studied under high-pressure continuous-flow conditions (200-250 degrees C, 30-40 bar), in the presence of micro/mesoporous zeotypes based on the MFI topology, which were prepared via different non-destructive bottom-up strategies: crystallization of silanized protozeolitic units; co-templating with a dual function (polymeric) template; and using a sole structure directing agent (non-surfactant and non-polymeric) to generate mesoporosity. The synthesis method influenced the material properties and consequently the catalytic performance. In targeting hydrocarbons with boiling point ranges characteristics of diesel, the zeotypes benefited from regular morphology, reduced crystallite size, mesoporosity and enhanced molar ratio of Lewis (L) to Bronsted (B) acid sites (L/B). In general, the zeotypes outperformed commercial zeolite ZSM-5. The best-performing zeotype was prepared according to the Serrano strategy based on the crystallization of silanized zeolitic seeds, and led to 97% conversion and an average space-time yield of liquid products of 1077 mg g(cat)(-1) h(-1), at 250 degrees C, 40 bar. The zeotypes seemed more stable than the commercial zeolite, based on molecular level characterization studies of the used/regenerated catalysts, with some differences in catalytic activity. (C) 2019 Elsevier Ltd. All rights reserved.
palavras-chave
QUALITY LIQUID FUELS; FISCHER-TROPSCH; PROPENE OLIGOMERIZATION; DIESEL PRODUCTION; ACID PROPERTIES; HIGH-PRESSURE; ZEOLITES; CATALYSTS; CONVERSION; ZSM-5
categoria
Science & Technology - Other Topics; Energy & Fuels
autores
Silva, AF; Fernandes, A; Antunes, MM; Ribeiro, MF; Silva, CM; Valente, AA
nossos autores
Anabela Tavares Aguiar Valente
Investigador Principal
Andreia de Freitas Silva
Bolseiro de investigação
Carlos Manuel Silva
Professor associado
Maria Margarida Feitor Pintão Moreno Antunes
Investigador Júnioragradecimentos
This work was developed in the scope of the project CICECO-Aveiro Institute of Materials, FCT (Fundacao para a Ciencia e Tecnologia) Ref. UID/CTM/50011/2019, financed by national funds through the FCT/MOTES. The FCT and the European Union are acknowledged for a Ph.D. grant to A.F.S. (SFRH/BD/101018/2014). M.M.A. and A.F. thank the costs resulting from the FCT hirings which are funded by national funds (OE), through FCT - Fundacao para a Ciencia e a Tecnologia, I.P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of the article 23, of the Decree-Law 57/2016, of August 29, changed by Law 57/2017, of July 19. The authors wish to thank Saint-Gobain Ceramic Materials AS for generously supplying the SIKA SiC sample.