Mesostructured Catalysts Based on the BEA Topology for Olefin Oligomerisation

resumo

Mesostructured solid acid catalysts based on the BEA topology were explored for olefin oligomerisation, which is an attractive synthetic route to produce clean, sulfur-free fuels or fuel additives with reduced aromatics content. Specifically, the oligomerisation of 1-butene, which may derive from (non-)renewable sources, was performed under high pressure and continuous-flow operation. The mesostructured catalysts consisted of a hierarchical zeotype (BEA-hier) synthesized by a one-pot approach using a dual-function template and, on the other hand, a composite (BEA/TUD) possessing zeolite nanocrystallites embedded in a mesoporous matrix synthesised under hydrothermal conditions. The influence of the material properties, catalyst activation temperature and reaction parameters were investigated by combining characterisation, two-dimensional gas chromatography combined with time-of-flight mass spectrometry (ToFMS) studies, and catalytic studies. The catalytic performances were compared to those of commercial nano/microcrystalline zeolites of different topologies and COD-900 (type of catalyst for the conversion of olefins to distillates process). BEA-hier performed superiorly in terms of conversion and space-time yields to diesel cut products.

palavras-chave

HIERARCHICAL MESOPOROUS ZEOLITES; FISCHER-TROPSCH; AL-27 MAS; ALKENE OLIGOMERIZATION; ACID PROPERTIES; BETA-ZEOLITE; DIESEL FUELS; H-BETA; ISOBUTENE; NMR

categoria

Chemistry

autores

Silva, AF; Fernandes, A; Neves, P; Antunes, MM; Rocha, SM; Ribeiro, MF; Silva, CM; Valente, AA

nossos autores

agradecimentos

This work was developed in the scope of the project (Associate Laboratory) CICECO Aveiro Institute of Materials-POCI-01-0145-FEDER-007679 [FCT (Fundacao para a Ciencia e a Tecnologia) ref. UID/CTM/50011/2013], and QOPNA research Unit (FCT UID/QUI/00062/2013), financed by national funds through the FCT/MEC and when applicable co-financed by FEDER (Fundo Europeu de Desenvolvimento Regional) under the PT2020 Partnership Agreement. The FCT and the European Union are acknowledged for a Ph.D. grant to A.F.S. (SFRH/BD/101018/2014), and post-doctoral grants to A.F (SFRH/BPD/91397/2012), P.N. (SFRH/BPD/110530/2015) and M.A. (SFRH/BPD/89068/2012), co-funded by MCTES and the European Social Fund through the program POPH of QREN. The authors wish to thank Saint-Gobain Ceramic Materials AS for generously supplying the SIKA SiC sample, and to Clariant Produkte GmbH, Germany for generously supplying the COD-900 sample.

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