This study highlights new opportunities for optimal reaction route selection from large chemical databases brought about by the rapid digitalisation of chemical data. The chemical industry requires a transformation towards more sustainable practices, eliminating its dependencies on fossil fuels and limiting its impact on the environment. However, identifying more sustainable process alternatives is, at present, a cumbersome, manual, iterative process, based on chemical intuition and modelling. We give a perspective on methods for automated discovery and assessment of competitive sustainable reaction routes based on renewable or waste feedstocks. Three key areas of transition are outlined and reviewed based on their state-of-the-art as well as bottlenecks: (i) data, (ii) evaluation metrics, and (iii) decision-making. We elucidate their synergies and interfaces since only together these areas can bring about the most benefit. The field of chemical data intelligence offers the opportunity to identify the inherently more sustainable reaction pathways and to identify opportunities for a circular chemical economy. Our review shows that at present the field of data brings about most bottlenecks, such as data completion and data linkage, but also offers the principal opportunity for advancement.

Data-driven models are becoming increasingly popular in engineering, on their own or in combination with mechanistic models. Commonly, the trained models are subsequently used in model-based optimization of design and/or operation of processes. Thus, it is critical to ensure that data-driven models are not evaluated outside their validity domain during process optimization. We propose a method to learn this validity domain and encode it as constraints in process optimization. We first perform a topological data analysis using persistent homology identifying potential holes or separated clusters in the training data. In case clusters or holes are identified, we train a one-class classifier, i.e., a one-class support vector machine, on the training data domain and encode it as constraints in the subsequent process optimization. Otherwise, we construct the convex hull of the data and encode it as constraints. We finally perform deterministic global process optimization with the data-driven models subject to their respective validity constraints. To ensure computational tractability, we develop a reduced-space formulation for trained one-class support vector machines and show that our formulation outperforms common full-space formulations by a factor of over 3000, making it a viable tool for engineering applications. The method is ready-to-use and available open-source as part of our MeLOn toolbox (https://git.rwth-aachen.de/avt.svt/public/MeLOn).

Optimal reaction pathways for the conversion of renewable feedstocks are often examined by reaction network flux analysis. An alternative modelling approach for reaction networks is a Petri net. These explicitly take the reaction sequence into account. In the optimisation of a network, this can allow the implementation of constraints on circular reaction structures, which are common substructures in chemical reaction networks. In this study, we compare the performance of the models in an illustrative minimal working example of a circular reaction substructure. The reaction network flux analysis is shown to be a relaxation of the Petri net formulation. Most notable, this work contributes to well-reasoned model choices for reaction networks.