One-pot gas-phase upgrading of low-carbon alcohols and acetone to C2-C8 olefins on Zn-Zr oxides

IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Chemical Engineering Science Pub Date : 2025-06-15 Epub Date: 2025-04-19 DOI:10.1016/j.ces.2025.121705
Cristhian A. Fonseca Benítez, Pablo J. Luggren
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Abstract

ABE (acetone-butanol-ethanol) and IBE (isopropanol-butanol-ethanol) fermentation are well-established processes for producing ketones and alcohols from biomass. Using these low-carbon alcohols and acetone might improve the production of olefins.
The gas-phase synthesis of light olefins from 1-butanol, ABE and IBE was investigated on Zn-Zr mixed oxides and reference ZnO and ZrO2. Zn-Zr catalysts with different Zn/Zr molar ratios (0.11–0.43) were prepared by incipient wetness impregnation of Zn on Zr(OH)4. The 1-butanol to olefin reaction pathways operating under different reaction conditions were elucidated. This tandem process comprises dehydrogenation, ketonization, aldol condensation, C–C bond cleavage, and deoxygenation reactions. ABE and IBE mixtures conversion was also evaluated, achieving total olefin yields of ∼65 %. Isobutene and ethylene (∼91 %) were the main components of the olefin fraction, while pentenes, isohexenes, heptenes, and octenes were the remaining components. These results highlight the potential of Zn-Zr oxides to develop a sustainable production of olefins.

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低碳醇和丙酮在Zn-Zr氧化物上一锅气相提质制C2-C8烯烃
ABE(丙酮-丁醇-乙醇)和IBE(异丙醇-丁醇-乙醇)发酵是从生物质中生产酮和醇的成熟工艺。使用这些低碳醇和丙酮可以提高烯烃的产量。以Zn-Zr混合氧化物和参比ZnO和ZrO2为原料,研究了1-丁醇、ABE和IBE气相合成轻烯烃的工艺。采用Zn在Zr(OH)4上的初湿浸渍法制备了不同Zn/Zr摩尔比(0.11 ~ 0.43)的Zn-Zr催化剂。阐明了不同反应条件下1-丁醇制烯烃的反应途径。该串联过程包括脱氢、酮化、醛缩、C-C键裂解和脱氧反应。还对ABE和IBE混合物的转化率进行了评估,总烯烃收率为~ 65 %。异丁烯和乙烯(~ 91 %)是烯烃组分的主要成分,其余组分为戊烯、异己烯、庚烯和辛烯。这些结果突出了Zn-Zr氧化物在烯烃可持续生产方面的潜力。
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来源期刊
Chemical Engineering Science
Chemical Engineering Science 工程技术-工程:化工
CiteScore
7.50
自引率
8.50%
发文量
1025
审稿时长
50 days
期刊介绍: Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.
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