Selective Preparation of Light Olefins from Cellulose-Derived Fermentation Intermediates
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Abstract: Directional synthesis of bio-based light olefins has great significance for promoting sustainable development of chemical industry. Present work proves that light olefins can be selectively prepared from the cellulose-derived acetone-butanol-ethanol. This transformation has been achieved by coupling cellulose fermentation and acetone-butanol-ethanol catalytic dehydration over the Ce@SAPO-34 catalyst. The active sites and reusability of the catalyst were investigated. High acetone-butanol-ethanol conversion (91.9%) and high olefin selectivity (86.1%) are achieved. Based on the study of the individual components in acetone-butanol-ethanol, the reaction pathways are put forward.
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Figure 1. Influence of temperature on production of light-olefins from dehydrated ABE. Reaction conditions: 2 g Ce/SAPO34 catalyst, 2 g dehydrated ABE. (a) conversion, olefin yield, olefin selectivity, and carbon balance; (b) selectivity of different products.
Figure 2. Production of light olefins from two cellulose derived ABE. (a) aqueous ABE (water content: 97.8%); (b) dehydrated ABE (water content: 5.8%). Reaction conditions: 2 g Ce/SAPO34 catalyst, 2 g ABE, T=350 °C.
Figure 3. Catalyst characterization of Ce/SAPO-34 catalyst. (a) N2 adsorption-desorption isotherms, (b) pore distribution, (c) SEM image, (d) TEM image.
Figure 4. Possible reaction pathways for production of light olefins from cellulose-based ABE.
Figure 5. Catalyst stability and reusability in the production of light olefins from the dehydrated ABE. Reaction condition: 2 g Ce/SAPO34 catalyst, 2 g dehydrated ABE, T=350 °C. Regeneration condition: T=550 °C, t=2 h. (a) Conversion, olefin yield and carbon balance, (b) selectivity of different products.
Table I. Production of light-olefins from the dehydrated ABE using different catalysts. C: conversion, Solefin: olefin selectivity, Saromatics: aromatics selectivity, and Yolefin: olefin yield. Reaction conditions: 2 g catalyst, 2 g dehydrated ABE, T=350 °C.
Catalysts C/% Solefin/% Saromatics/% Yolefin/% Al-MCM-41 89.5 49.9 19.2 44.7 HZSM-5 92.5 51.5 24.5 47.6 Ce/SAPO-34 91.9 86.1 4.4 79.1 SAPO-34 93.2 82.7 6.5 77.1 Hβ 90.8 56.6 20.2 51.4 
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Table II. Main characteristics of catalysts. SBET: Brunauer-Emmet-Teller surface area in m2/g, Vp: pore-volume in cm3/g, Total acidity in µmol NH3/g, B/L: Bronsted/Lewis acid ratio and S/W: strong/weak acid ratio.
Catalysts SBET Vp Total acidity B/L S/W HZSM-5 455 0.22 580 5.5 0.9 Hβ 608 0.31 303 0.4 0.7 Al-MCM-41 1020 0.52 264 1.7 0.3 SAPO-34 592 0.30 1393 0.6 Ce@SAPO-34 408 0.18 1027 0.3
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