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Selective Production of Glycolaldehyde via Hydrothermal Pyrolysis of Glucose: Experiments and Microkinetic Modeling
Journal of Analytical and Applied Pyrolysis ( IF 6 ) Pub Date : 2020-08-01 , DOI: 10.1016/j.jaap.2020.104846
Pavlo Kostetskyy , Matthew W. Coile , Joshua M. Terrian , Jake W. Collins , Kevin J. Martin , James F. Brazdil , Linda J. Broadbelt

Abstract Pyrolysis of glucose and glucose-based carbohydrates has been shown to produce a range of chemical species that can be used directly as fuels and chemicals or as feedstocks to further chemical transformations. It is known that process operating conditions such as temperature, heating rate, reactor configuration, moisture content, and pretreatment method can have a significant effect on the observed product distribution. Pyrolysis of carbohydrates in the presence of water at high concentrations can significantly alter the product spectrum and favor the production of specific products at unusually high yields. In this work, we show that pyrolysis of aqueous glucose solutions at high temperatures can result in highly selective production of glycolaldehyde, a C2 hydrocarbon with an aldehyde and hydroxyl functionality, toward direct applications in the food industry or as a chemical building block toward value-added products. A glucose pyrolysis model that was developed previously was expanded to capture the pyrolysis kinetics of glucose at hydrothermal conditions, accurately reproducing the observed product yields for a range of temperatures and feedstock compositions. Dominant reaction families were identified and interrogated to quantify the effect of hydrothermal conditions on the predicted kinetics. High yields of glycolaldehyde were achieved experimentally, with the maximum values observed at moderate temperatures and pure glucose feed. Elevated temperatures and increasing fructose concentrations negatively affected observed glycolaldehyde yields, resulting in increased production of undesired decomposition products in the C1-C3 range. The results of this study include preferred operating conditions toward maximizing the yield of glycolaldehyde as described by a predictive kinetic model that explicitly accounts for the major reactions comprising a complex network taking place and the effect of the operating conditions on their relative contributions to glucose conversion and product yields.

中文翻译:

通过葡萄糖的水热热解选择性生产乙醇醛:实验和微动力学建模

摘要 葡萄糖和基于葡萄糖的碳水化合物的热解已被证明可产生一系列化学物质,这些物质可直接用作燃料和化学品或用作进一步化学转化的原料。众所周知,工艺操作条件,如温度、加热速率、反应器配置、水分含量和预处理方法,会对观察到的产品分布产生重大影响。在高浓度水存在下碳水化合物的热解可以显着改变产品谱并有利于以异常高的产率生产特定产品。在这项工作中,我们表明在高温下葡萄糖水溶液的热解可以导致乙醇醛的高度选择性生产,乙醇醛是一种具有醛和羟基官能团的 C2 烃,直接应用于食品工业,或作为化学基础材料用于增值产品。先前开发的葡萄糖热解模型被扩展以捕获葡萄糖在水热条件下的热解动力学,准确再现观察到的一系列温度和原料组成的产品产量。确定并询问了主要反应族,以量化水热条件对预测动力学的影响。通过实验实现了乙醇醛的高产率,在中等温度和纯葡萄糖进料下观察到最大值。升高的温度和增加的果糖浓度对观察到的乙醇醛产率产生负面影响,导致 C1-C3 范围内不希望的分解产物的产生增加。
更新日期:2020-08-01
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