Arnab Chaudhuri, Wouter F.C. de Groot, Jasper H.A. Schuurmans, Stefan D.A. Zondag, Alessia Bianchi, Koen P.L. Kuijpers, Rémy Broersma, Amin Delparish, Matthieu Dorbec, John van der Schaaf, Timothy Noël
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引用次数: 0
摘要
在过去的十年中,光化学转化因其能够在温和的条件下实现独特的反应而重新引起了人们的兴趣。然而,扩大这种工艺的规模,特别是在多相系统(如气液)中,仍然具有挑战性。先前,我们证明了光化学转子-定子旋转圆盘反应器(pRS-SDR)在α-萜烯光氧化转化为天冬酰胺方面的潜力,尽管该系统受到光源的限制,导致在光子有限的情况下运行不理想。在这项工作中,我们通过集成专门为反应器设计的高功率光源(高达652w光输出)来释放pRS-SDR的全部潜力。结果表明,在高辐照度下,pRS-SDR可以实现高气液传质率,从而显著提高生产率(α-萜烯转化率为92%时为16.3 kg day-1,在27 mL辐照体积内为2.52 W cm-2),与我们之前的研究相比,提高了一个数量级。然而,β-香茅醇的光氧化表现出明显的局限性,这突出了在评估强化光化学反应器时选择合适的模型反应的重要性。
Scaling Up Gas–Liquid Photo-Oxidations in Flow Using Rotor-Stator Spinning Disc Reactors and a High-Intensity Light Source
Photochemical transformations have garnered renewed interest over the past decade for their ability to enable unique reactions under mild conditions. However, scaling up such processes, particularly in multiphase systems (e.g., gas–liquid), remains challenging. Previously, we demonstrated the potential of the photochemical rotor-stator spinning disc reactor (pRS-SDR) for scaling the photooxidation of α-terpinene to ascaridole, though the system was limited by the light source, resulting in suboptimal operation in a photon-limited regime. In this work, we unlock the full potential of the pRS-SDR by integrating a high-powered light source (up to 652 W optical output) specifically designed for the reactor. The results show that the high gas–liquid mass transfer rates achievable in the pRS-SDR allow for significant productivity improvements under high irradiance (16.3 kg day–1 at 92% α-terpinene conversion and 2.52 W cm–2 in a 27 mL irradiated volume), representing an order of magnitude increase compared to our previous study. However, the photooxidation of β-citronellol exhibited notable limitations, highlighting the importance of selecting appropriate model reactions when evaluating intensified photochemical reactors.
期刊介绍:
The journal Organic Process Research & Development serves as a communication tool between industrial chemists and chemists working in universities and research institutes. As such, it reports original work from the broad field of industrial process chemistry but also presents academic results that are relevant, or potentially relevant, to industrial applications. Process chemistry is the science that enables the safe, environmentally benign and ultimately economical manufacturing of organic compounds that are required in larger amounts to help address the needs of society. Consequently, the Journal encompasses every aspect of organic chemistry, including all aspects of catalysis, synthetic methodology development and synthetic strategy exploration, but also includes aspects from analytical and solid-state chemistry and chemical engineering, such as work-up tools,process safety, or flow-chemistry. The goal of development and optimization of chemical reactions and processes is their transfer to a larger scale; original work describing such studies and the actual implementation on scale is highly relevant to the journal. However, studies on new developments from either industry, research institutes or academia that have not yet been demonstrated on scale, but where an industrial utility can be expected and where the study has addressed important prerequisites for a scale-up and has given confidence into the reliability and practicality of the chemistry, also serve the mission of OPR&D as a communication tool between the different contributors to the field.