Multi-objective optimisation: algorithms and application to computer-aided molecular and process design

Computer-Aided Molecular Design (CAMD) has been put forward as a powerful and systematic technique that can accelerate the identification of new candidate molecules. Given the benefits of CAMD, the concept has been extended to integrated molecular and process design, usually referred to as Computer-Aided Molecular and Process Design (CAMPD). In CAMPD approaches, not only is the interdependence between the properties of the molecules and the process performance captured, but it is also possible to assess the optimal overall performance of a given fluid using an objective function that may be based on process economics, energy efficiency, or environmental criteria. Despite the significant advances made in the field of CAM(P)D, there are remaining challenges in handling the complexities arising from the large mixed-integer nonlinear structure-property and process models and the presence of conflicting performance criteria that cannot be easily merged into a single metric. Many of the algorithms proposed to date, however, resort to single-objective decomposition-based approaches. To overcome these challenges, a novel CAMPD optimisation framework is proposed, in the first part of thesis, in the context of identifying optimal amine solvents for carbon dioxide (CO2) chemical absorption. This requires development and validation of a model that enables the prediction of process performance metrics for a wide range of solvents for which no experimental data exist. An equilibrium-stage model that incorporates the SAFT-γ Mie group contribution approach is proposed to provide an appropriate balance between accuracy and predictive capability with varying molecular design spaces. In order to facilitate the convergence behaviour of the process-molecular model, a tailored initialisation strategy is established based on the inside-out algorithm. Novel feasibility tests that are capable of recognising infeasible regions of molecular and process domains are developed and incorporated into an outer-approximation framework to increase solution robustness. The efficiency of the proposed algorithm is demonstrated by applying it to the design of CO2 chemical absorption processes. The algorithm is found to converge successfully in all 150 runs carried out. To derive greater insights into the interplay between solvent and process performance, it is desirable to consider multiple objectives. In the second part of the thesis, we thus explore the relative performance of five multi-objective optimisations (MOO) solution techniques, modified from the literature to address nonconvex MINLPs, on CAM(P)D problems to gain a better understanding of the performance of different algorithms in identifying the Pareto front efficiently. The combination of the sandwich algorithm with a multi-level single-linkage algorithm to solve nonconvex subproblems is found to perform best on average. Next, a robust algorithm for bi-objective optimisation (BOO), the SDNBI algorithm, is designed to address the theoretical and numerical challenges associated with the solution of general nonconvex and discrete BOO problems. The main improvements in the development of the algorithm are focused on the effective exploration of the nonconvex regions of the Pareto front and the early identification of regions where no additional Pareto solutions exist. The performance of the algorithm is compared to that of the sandwich algorithm and the modified normal boundary intersection method (mNBI) over a set of literature benchmark problems and molecular design problems. The SDNBI found to provide the most evenly distributed approximation of the Pareto front as well as useful information on regions of the objective space that do not contain a nondominated point. The advances in this thesis can accelerate the discovery of novel solvents for CO2 capture that can achieve improved process performance. More broadly, the modelling and algorithmic development presented extend the applicability of CAMPD and MOO based CAMD/CAMPD to a wider range of applications.Open Acces