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

目的：该项目将使用工业4.0平台开发新型贱金属催化工艺，结合在线分析和算法控制，随后从产品中电化学去除金属。加强对贱金属催化的理解和控制将使人们能够摆脱贵金属，而电化学回收/再循环则使制药和农业化学产品的原子效率更高。方法：1.在电化学连续流平台内集成和优化在线分析，用于贱金属催化的合成和评估。这将涉及对平台进行初步的“概念验证”评估，其中包括已建立的、易于获得的催化剂或盐，并逐步发展为工业相关的催化剂。在此之后，将进行工业相关催化剂合成的研究和工业相关工艺的后续评价。2.原位贱金属（催化剂）去除方案的开发。这将需要建立电化学反应废物和整个贱金属催化过程的初步发展。随后，将使用一系列贱金属研究开发的方案的应用，从而进行去除贵金属（Pd/ Rd）的比较研究。在与工业赞助商进行安置期间，有可能将该议定书适用于工业废物流，有待讨论。3.开发一种特定于应用的自优化算法，可以有效地探索电化学流动平台的操作条件，以获得最大限度地提高工艺生产率、鲁棒性和可持续性的条件。这将涉及通过结合绿色指标和催化剂指标开发现有算法，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用于反应建模，以告知工艺控制/优化（例如，电极上的金属、配体结合/释放部位;反应器内的流动状态）。影响：行业标准反应筛选平台--通过在行业中的潜在吸收、通过期刊出版物以及通过其他人来利兹使用该平台筛选他们感兴趣的反应的潜力产生影响。加强对贱金属催化工艺的理解-通过工业工艺变得更有效率和/或逐步放弃贵金属以及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-通过更有效/更低成本地去除金属，通过回收/再利用提高原子效率，从而产生潜在的工业影响。预期可实现性：在电化学连续流平台内集成和优化在线分析，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。开发原位贱金属（催化剂）去除方案。开发特定应用的自优化算法，可有效探索电化学流动平台的操作条件，以获得最大化工艺生产率、稳健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.