Inert Atmosphere Automated Synthesis for the Investigation of Nuclear Waste relevant species (DIGINERT)

预计在下个世纪，管理英国的核遗产将耗资1240亿英镑，其中很大一部分来自处理和处置高放射性锕系元素废物，如钚和铀。这些放射性物质的人工处理和化学操作对工业来说是一项危险的任务，需要实施极其昂贵的风险缓解措施。许多锕系元素在与空气接触时可能点燃，这进一步增加了风险，这意味着必须使用技术来防止它们暴露于氧气和水分中。最近，自动化工具越来越多地纳入化学家的工作流程，提高了安全性和吞吐量，同时减少了时间和劳动力成本。然而，在这些系统中有一种试剂是恒定的，那就是空气。这种反应性气体对化学的影响是不可低估的，通过提供干燥的环境，可以在惰性或不同的气氛下进行实验，从而可以获得大量未被发现的科学。重要的是，将可远程操作的自动化工具用于锕系元素处理，可以大大提高研究人员的安全性，降低核工业的成本，同时使我们能够缩小目前存在于这些难以探测的材料行为的相当大的知识差距。在这项研究中，我将开发第一个在没有空气和水分的情况下进行化学操作的综合自动化技术，并将与塞拉菲尔德核基地合作，开发用于关键惰性操作远程自动化的安全工具。这项工作建立在我在锕系元素科学和无机化学自动化方面的记录之上，但也进一步推动了满足工业需求的工具的建立。该项目有三个关键步骤：构建，安全和验证。我将首先建立一套技术，使全反应自动化，同时排除空气和水，允许在不同的气体条件下进行广泛的化学反应。首先，将开发一种低成本的远程操作气体和真空分配系统，该系统允许多个反应堆系统地净化空气和水，以及一系列数字可控的气密反应堆，用于安全储存和运输高活性物质。我还将开发一种集成气液处理系统，提高惰性条件下反应的安全性和吞吐量。通过设计厌氧处理系统，我将提高我们能够在惰性条件下研究不同反应的速度。接下来，我将制定新的策略来确保安全自动化。我将与传感器设计方面的专家合作，在技术中建立反馈，作为潜在危险的早期检测系统，包括压力增加、温度升高和辐射泄漏。我还将开发新的风险评估技术，这些技术可以标记潜在的危险，并提前提出缓解措施的建议。本文开发的技术将在铀化合物的合成上进行验证，作为核废料行为的模型。铀亚胺配合物可以作为存在于核废料中的锕系氧的可溶性类似物，并允许我们深入探索这些物种的行为。利用我的惰性气氛技术，模型配合物将被合成，随后使用上述技术与一系列相关污染物（如H2）反应。最后，在整个项目中，我将与Sellafield的科学家密切合作。我们将一起设计实验，以应对他们的关键挑战，并展示我的技术对行业的实用性。我还将利用这个奖学金机会加深我在工业界的联系，并努力使我的技术在英国适当的地点得到实施和处理放射性物质。

Managing the UKs nuclear legacy is projected to cost £124B over the next century, a large portion of which derives from handling and disposal of highly radioactive actinide wastes, such as plutonium and uranium. Manual handling and chemical manipulation of these radioactive materials presents a hazardous task for the industry and requires extremely costly risk mitigation measures to be implemented. The risk is increased further by the potential of many actinide species to ignite on contact with air, meaning technologies must be used to prevent their exposure to oxygen and moisture.Recently, automation tools have increasingly been incorporated into a chemist's workflow, improving safety and throughput while decreasing time and labor costs. However, one reagent is constant in these systems, air. The impact this reactive gas has on the chemistry cannot be understated and a wealth of undiscovered science is made available by providing dry environments which allow experiments to be conducted under inert or different atmospheres. Importantly, the incorporation of remotely operable automation tools for actinide handling could dramatically increase the safety of researchers and decrease costs in the nuclear industry, all while allowing us to narrow the sizeable knowledge gap which currently exists for the behavior of these difficult to probe materials.In this Fellowship I will develop the first comprehensive automation technology for chemical manipulations in the absence of air and moisture and will collaborate with Sellafield nuclear site to develop safe tools for the remote automation of key inert operations. This work builds upon my track record in actinide science and automation of inorganic chemistry but also pushes further towards building tools which meet industrial needs.This project has three key steps: Build, Secure & Validate.I will first build a suite of technologies which allow automation of full reactions while excluding air and water allowing for a wide range of chemistry to be undertaken under different gas conditions. Firstly a low-cost remotely operable gas & vacuum distribution system will be developed which allows multiple reactors to be systematically purged of air and water along with a range of digitally controllable air-tight reactors for the safe storage and transportation of highly reactive species. I will also develop an integrated gas-liquid handing system increasing both safety and throughput of reactions under inert conditions. By designing the system with anaerobic handling in mind I will increase the speed at which we are able to investigate different reactions under inert conditions.Next, I will develop new strategies to ensure safe automation. I will collaborate with experts in sensor design to build feedback into the technology as an early detection system for potential hazards including pressure increases, elevated temperature and radiation leaks. I will also develop new risk assessment technologies which can flag potential hazards and suggest mitigation steps in advance.The technology developed herein will be validated on the synthesis of uranium compounds as models of nuclear waste materials behavior. Uranium imido complexes which can act as soluble analogues of the actinide oxo species present in nuclear wastes and allow us to deeply probe the behavior of these species. Utilizing my inert atmosphere technologies model complexes will be synthesized and subsequently reacted with a range of relevant contaminants (eg H2) using the technology described above.Finally, throughout this project I will collaborate closely with scientists as Sellafield. Together we will design experiments to meet their key challenges and demonstrate the utility of my technology for the industry. I will also build upon this Fellowship opportunity to deepen my ties within industry and work towards having my technologies implemented & handling radioactive materials at an appropriate UK site.