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Optimization of continuous-flow heterogeneous catalytic oligomerization of 1-butene by design of experiments and response surface methodology

机译：通过实验和响应面法设计优化1-丁烯的连续流非均相催化齐聚

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Oligomerization of light olefins allows the production of clean, sulphur-free fuels or fuel additives with reduced aromatics content, and useful chemicals. Commercial heterogeneous catalytic oligomerization technologies were developed to meet market demands in flexible fashions, whereby the operating conditions may be adjusted in favor of the desired product specifications and yields. For achieving superior performances, the development of expeditious evaluation and optimization tools is important, albeit not trivial because light olefins oligomerization involves complex reaction systems and product quality depends on many factors. In this sense, the design of experiments (DoE) and response surface methodology (RSM) are valuable tools, yet unexploited for light olefins oligomerization processes. In this work, DoE/RSM models were developed and validated for the oligomerization of 1-butene - derivable from fossil or renewable sources of organic carbon - over a superior hierarchical zeotype catalyst, under high pressure, continuous flow conditions, targeting clean diesel range products. The models allowed to investigate the individual and cross effects of reaction pressure, temperature and weight hourly space velocity on conversion and yields of specific product fractions. The optimization studies also accounted for product quality features such as, reduced aromatics content; these studies counted with the analytical input of Comprehensive Two-Dimensional Gas Chromatography with Time-of-Flight Mass Spectrometry (GC x GC-ToEMS) for characterizing the products. Importantly, DoE/RSM tools may contemplate not only kinetic data, but also product quality indicators, and help identify most relevant process parameters impacting on the productivity.
机译：轻质烯烃的低聚可生产清洁的，无硫的燃料或芳香烃含量降低的燃料添加剂和有用的化学物质。已开发出商业上的非均相催化低聚技术，以灵活的方式满足市场需求，由此可以调节操作条件以有利于所需的产品规格和产率。为了获得优异的性能，开发快速的评估和优化工具非常重要，尽管这并非轻而易举，因为轻烯烃的低聚反应涉及复杂的反应系统，并且产品质量取决于许多因素。从这个意义上讲，实验设计（DoE）和响应面方法（RSM）是有价值的工具，但尚未用于轻烯烃低聚过程。在这项工作中，开发了DoE / RSM模型，并在高压，连续流动条件下，在高级连续型催化剂上，针对1-丁烯（可从化石或可再生有机碳来源衍生）的低聚反应进行了验证，以清洁柴油系列产品为目标。该模型允许研究反应压力，温度和重量时空速度对特定产物级分的转化率和产率的个体和交叉影响。优化研究还考虑了产品质量特征，例如降低的芳烃含量；这些研究都用具有飞行时间质谱的综合二维气相色谱（GC x GC-ToEMS）的分析输入来表征产品。重要的是，DoE / RSM工具不仅可以考虑动力学数据，还可以考虑产品质量指标，并帮助确定影响生产率的最相关的过程参数。

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