Molecular engineering of sustainable phase-change solvents: From digital design to scaling-up for CO2 capture

[Display omitted] •Digital design and experimental validation of phase-change CO2 capture solvents.•Evaluation of thermodynamics, reactivity, process and sustainability properties.•SAFT-γ Mie predicts entire three-phase envelope for S1N/DMCA + H2O + CO2.•Low regeneration energy, viscosity and vapour losses, high cyclic capacity.•Favourable health and safety performance compared to other solvents. Phase-change solvents promise reduced energetic and environmental footprints for separation systems, including absorption-based CO2 abatement technologies. The search for efficient phase-change solvents is limited by challenges in vapour-liquid–liquid equilibrium (VLLE) prediction and in sustainability assessment. We overcome these with a digital approach to screen billions of structures and design the novel phase-change solvent S1N (N1-cyclohexylpropane-1,3-diamine) and mixture S1N/DMCA (N,N-dimethylcyclohexylamine). Screening criteria include thermodynamic and process-related properties, reactivity and sustainability of solvent production and use. VLLE phase envelopes are predicted using the SAFT-γ Mie (Statistical Associating Fluid Theory) equation of state thanks to its transferability to any structure and the implicit modelling of ionic species. Experimental validation confirms the suitability of S1N/DMCA for scaling-up, with a cyclic capacity of 1.19 mol CO2/ kg-solvent, a regeneration energy of 2.3 GJ/ton-CO2, and vapour losses and viscosity lower by 10% and 70% than those of other solvents. S1N is also safer for plant operation and working personnel.