Potter Matthew E, Armstrong Lindsay-Marie, Carravetta Marina, Mezza Thomas M, Raja Robert
Faculty of Engineering and Physical Sciences, University of Southampton, Southampton, United Kingdom.
UOP, A Honeywell Company, Des Plaines, IL, United States.
Front Chem. 2020 Mar 17;8:171. doi: 10.3389/fchem.2020.00171. eCollection 2020.
The introduction of two distinct dopants in a microporous zeotype framework can lead to the formation of isolated, or complementary catalytically active sites. Careful selection of dopants and framework topology can facilitate enhancements in catalysts efficiency in a range of reaction pathways, leading to the use of sustainable precursors (bioethanol) for plastic production. In this work we describe our unique synthetic design procedure for creating a multi-dopant solid-acid catalyst (MgSiAPO-34), designed to improve and contrast with the performance of SiAPO-34 (mono-dopant analog), for the dehydration of ethanol to ethylene. We employ a range of characterization techniques to explore the influence of magnesium substitution, with specific attention to the acidity of the framework. Through a combined catalysis, kinetic analysis and computational fluid dynamics (CFD) study we explore the reaction pathway of the system, with emphasis on the improvements facilitated by the multi-dopant MgSiAPO-34 species. The experimental data supports the validation of the CFD results across a range of operating conditions; both of which supports our hypothesis that the presence of the multi-dopant solid acid centers enhances the catalytic performance. Furthermore, the development of a robust computational model, capable of exploring chemical catalytic flows within a reactor system, affords further avenues for enhancing reactor engineering and process optimisation, toward improved ethylene yields, under mild conditions.
在微孔沸石型骨架中引入两种不同的掺杂剂可导致形成孤立的或互补的催化活性位点。仔细选择掺杂剂和骨架拓扑结构有助于提高一系列反应途径中催化剂的效率，从而能够使用可持续的前体（生物乙醇）来生产塑料。在这项工作中，我们描述了一种独特的合成设计程序，用于制备一种多掺杂固体酸催化剂（MgSiAPO-34），该催化剂旨在改善乙醇脱水制乙烯的性能，并与SiAPO-34（单掺杂类似物）的性能形成对比。我们采用一系列表征技术来探究镁取代的影响，特别关注骨架的酸度。通过联合催化、动力学分析和计算流体动力学（CFD）研究，我们探索了该体系的反应途径，重点是多掺杂MgSiAPO-34物种所带来的改进。实验数据支持了在一系列操作条件下CFD结果的有效性；这两者都支持了我们的假设，即多掺杂固体酸中心的存在提高了催化性能。此外，开发一个能够探索反应器系统内化学催化流的强大计算模型，为在温和条件下提高乙烯产率，进一步优化反应器工程和工艺提供了更多途径。
