resumo
Solid acid catalysts possessing MFI topology and different crystal sizes and porosities were explored for the conversion of carbohydrate-biomass- derived alpha-angelica lactone and 5-(hydroxymethyl) furfural, in 1-butanol at T= 120-170 degrees C, to give levulinate esters and furanic ethers. Micro/mesoporous microcrystalline catalysts were prepared by post-synthesis base/acid treatments of ZSM-5 zeolite; the influence of the desilication (base) conditions on the material properties was investigated. A nanocrystalline ZSM-5 sample was synthesised by using hydrothermal, dynamic conditions and used as a reference material. A comparison of the catalytic performances of materials featuring different morphological, textural, and acid properties highlights a complex interplay between the acid and textural properties. The best-performing catalyst (MZS0.6) was obtained by post-synthesis-treatment; fairly good catalytic stability was confirmed by catalyst recycling, contact tests, and characterisation of the spent catalyst. MZS0.6 was compared with the macrorecticular ion-exchange resin Amberlyst-15, chosen as a benchmark solid acid catalyst, in the two reaction systems.
palavras-chave
MESOPOROUS ZSM-5 ZEOLITES; RENEWABLE LEVULINIC ACID; ACTIVE SULFATED ZIRCONIA; ETHYL LEVULINATE; TRANSFER HYDROGENATION; HIERARCHICAL ZSM-5; NAOH/TETRABUTYLAMINE HYDROXIDE; LIGNOCELLULOSIC BIOMASS; DESILICATED ZSM-5; FURFURYL ALCOHOL
categoria
Chemistry
autores
Antunes, MM; Lima, S; Fernandes, A; Magalhaes, AL; Neves, P; Silva, CM; Ribeiro, MF; Chadwick, D; Hellgardt, K; Pillinger, M; Valente, AA
nossos autores
Ana Luísa Carvalho Magalhães
Bolseiro de pós-Doutoramento
Anabela Tavares Aguiar Valente
Investigador Principal
Carlos Manuel Silva
Professor associado
Maria Margarida Feitor Pintão Moreno Antunes
Investigador Júnior
Martyn Pillinger
Investigador Principal
Patrícia dos Santos Neves
Investigador Auxiliaragradecimentos
This work was developed in the scope of the project CICECO-Aveiro Institute of Materials, POCI-01-0145-FEDER-007679 (FCT ref. UID/CTM/50011/2013), financed by national funds through the FCT/MEC and co-financed by FEDER under the PT2020 Partnership Agreement. The FCT and the European Union are acknowledged for postdoctoral grants to M.M.A. (SFRH/BPD/89068/2012), A.F. (SFRH/BPD/91397/2012), A.L.M. (SFRH/BPD/95393/2013), and P.N. (SFRH/BPD/73540/2010), co-funded by MCTES and the ESF through the program POPH of QREN. S.L., K.H., and D.C. thank EPSRC (UK) for financial support under EP/K014749/1. The authors are grateful to Dr. Rosario Soares (CICECO) for assistance with the powder XRD measurements and data processing.