Catalytic oxidation of aqueous bioethanol: an efficient upgrade from batch to flow†,Reaction Chemistry & Engineering

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Catalytic oxidation of aqueous bioethanol: an efficient upgrade from batch to flow†
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2018-08-28 00:00:00 , DOI: 10.1039/c8re00054a
Sotiria Mostrou _{1,

2,

3,

4,

5} , Tamás Sipőcz _{6,

7,

8,

9,

10} , Andreas Nagl _{11,

12,

13,

14,

15} , Balázs Fődi _{6,

7,

8} , Ferenc Darvas _{6,

7,

8} , Karin Föttinger _{11,

12,

13,

14,

15} , Jeroen A. van Bokhoven _{1,

2,

3,

4,

5}

Affiliation

The heterogeneously catalyzed oxidation of (bio)ethanol to acetic acid is an environmentally friendly alternative to the current industrial Monsanto process. The reaction yields acetic acid from crude bioethanol under mild reaction conditions. The triphasic reaction is technically critical, due to mass and heat transfer limitations and is thus predominantly studied in batch reactor systems. However, in order to advance the industrial implementation of the catalytic route, the operation in flow at the research stage is necessary. It is an efficient, reliable, and safer system for triphasic reactions and allows us to define better performance parameters for a later up-scale of a continuous flow process. Here, we evaluated the aerobic ethanol oxidation in a flow reactor and compared it with a traditional batch system over a gold–titania catalyst under analogous conditions. In both reactors, the reaction mechanism was similar: there was a zero-order dependency in oxygen and a first-order dependency in ethanol. The different reaction orders indicate that oxygen and ethanol interact with different surface sites, possibly ethanol with gold and oxygen with the support. The study showed that the catalytic performance improves in flow by about 30% for conversion and by 10% for acetic acid selectivity. The enhancement is associated mainly with the greater resistance of gold to sintering in the flow reactor. The study underlines the necessity of switching research to flow systems in order to benchmark more efficiently and identify potential catalysts for industrial implementation as well as to enhance our understanding of triphasic reactions.

中文翻译：

水性生物乙醇的催化氧化：从批次到流量的有效升级†

（生物）乙醇多相催化氧化成乙酸是当前工业孟山都工艺的环保替代方案。在温和的反应条件下，该反应从粗制生物乙醇中产生乙酸。由于质量和传热的限制，三相反应在技术上很关键，因此主要在间歇反应器系统中进行了研究。然而，为了促进催化路线的工业实施，在研究阶段必须进行流动操作。它是用于三相反应的高效，可靠和安全的系统，使我们能够为后续的连续流工艺的更高规模定义更好的性能参数。这里，我们评估了流动反应器中的好氧乙醇氧化，并将其与在类似条件下在金-二氧化钛催化剂上的传统间歇系统进行了比较。在两个反应器中，反应机理都相似：氧的零级依赖性和乙醇的一级依赖性。不同的反应顺序表明，氧气和乙醇与不同的表面部位相互作用，可能是乙醇与金和氧气与载体相互作用。研究表明，催化性能将流动转化率提高了约30％，乙酸选择性提高了10％。增强主要与金在流动反应器中对烧结的更大抵抗力有关。

更新日期：2018-08-28

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