Development of base-metal catalysed processes using electrochemical generation and recovery/recycle of catalysts

目的：该项目将开发新的贱金属催化工艺，使用工业4.0平台，结合在线分析和算法控制，并随后从产品中电化学去除金属。加强对贱金属催化的了解和控制，将使人们能够摆脱贵金属，通过电化学回收/再循环，为制药和农用化学品产品提供更高效的原子途径。方法：1.整合和优化电化学连续流动平台中的在线分析，用于贱金属催化的合成和评价。这将包括对平台进行初步的“概念验证”评估，包括已建立的、容易获得的催化剂或盐，然后发展到与工业相关的催化剂。在此之后，将对工业相关催化剂的合成进行调查，并随后对工业相关工艺进行评估。2.开发了一种原位去除贱金属(催化剂)的方案。这将需要对已建立的电化学反应废物进行初步开发，并扩展到整个贱金属催化过程。随后，将对所制定的议定书在一系列贱金属中的应用进行调查，从而与贵金属(Pd/Rd)的去除进行对比研究。在与工业赞助商的安置期间，有可能将该议定书应用于工业废流，有待讨论。3.开发特定于应用的自我优化算法，该算法可以有效地探索电化学流平台的操作条件，以获得最大限度地提高工艺的生产率、健壮性和可持续性的条件。这将涉及通过纳入绿色指标和催化剂指标来开发现有算法，扩展到离散变量优化(例如，溶剂/金属盐、工艺/催化剂生命周期分析)。通过这些优化获得的数据将被提供给反应建模，以便为过程控制/优化提供信息(例如，金属、电极上的配体结合/释放的位置；反应器内的流动状态)。影响：行业标准的反应筛选平台-通过行业中的潜在吸收、通过期刊出版物以及通过其他人来到利兹使用该平台筛选他们感兴趣的反应的潜力而产生的影响。增进对贱金属催化过程的了解--通过工业过程变得更有效率和/或放弃贵金属和通过期刊出版物产生的影响。金属催化剂的电化学回收/再循环-通过更高效/更低成本地去除金属来潜在的工业影响，通过回收/再利用来提高原子效率。预期交付成果：整合和优化电化学连续流动平台内的在线分析，用于贱金属催化的合成和评估。在基准工业相关反应中电化学生成和筛选贱金属催化剂，以验证该平台。在更具挑战性的工业相关反应中电化学生成和筛选贱金属催化剂。开发一种原位去除贱金属(催化剂)的方案。开发特定于应用的自我优化算法，该算法可以有效地探索电化学流平台的操作条件，以获得最大限度地提高工艺的生产率、健壮性和可持续性的条件。

Aims: This project will result in the development of novel base-metal catalysed processes using an industry 4.0 platform combining in-line analysis and algorithm control, with subsequent electrochemical removal of the metal from the product. Enhanced understanding and control of base-metal catalysis will enable a move away from precious metals, with electrochemical recovery/recycle allowing a more atom-efficient route to pharmaceutical and agrochemical products. Methodology:1. The integration and optimisation of in-line analysis within an electrochemical continuous flow platform for the synthesis and evaluation of base-metal catalysis. This will involve initial 'proof of concept' evaluation of the platform with established, readily-available catalysts or salts, progressing to industrially relevant catalysts. Following this, investigation of industrially relevant catalyst synthesis and subsequent evaluation in industrially-relevant processes will be undertaken. 2. The development of an in situ base-metal (catalyst) removal protocol. This will require the initial development with established electrochemical reaction waste and telescoping with the entire base-metal catalysed process. Subsequently, application of the developed protocol will be investigated with a range of base metals, leading to comparative studies with removal of precious metals (Pd/ Rd). There is the potential to apply this protocol to industrial waste streams during a placement with an industrial sponsor, pending discussion. 3. The development of an application-specific self-optimisation algorithm that can efficiently explore operating conditions of the electrochemical flow platform, to obtain the conditions that maximises the process' productivity, robustness and sustainability. This will involve development of existing algorithms via the incorporation of green metrics and catalyst metrics, expanding to discrete variable optimisation (e.g. solvents/ metal salts, process/ catalyst lifecycle analysis). Obtained data through these optimisations will be provided for reaction modelling to inform process control/ optimisation (e.g. for sites of metal, ligand binding/release on electrode; flow regimes within reactor). Impact:Industry-standard reaction screening platform - impact through potential uptake in industry, through journal publications and through the potential for others to come to Leeds to use the platform to screen reactions that are of interest to them. Enhanced understanding of base-metal catalysed processes - impact through industrial processes becoming more efficient and/or a move away from precious metals and through journal publications. Electrochemical recovery/recycle of metal catalysts - potential industrial impact through more efficient/lower cost removal of metals, more atom efficiency through recovery/reuse. Expected Deliverables:Integration and optimisation of in-line analysis within an electrochemical continuous flow platform for the synthesis and evaluation of base-metal catalysis. Electrochemical generation and screening of base-metal catalysts in a benchmark industrially relevant reaction to validate the platform. Electrochemical generation and screening of base-metal catalysts in more challenging industrially relevant reactions. Development of an in situ base-metal (catalyst) removal protocol. Development of an application-specific self-optimisation algorithm that can efficiently explore operating conditions of the electrochemical flow platform, to obtain the conditions that maximises the process' productivity, robustness and sustainability.