A procedure is described for computer-assisted optimization of an electrolytic process flowsheet. Material, energy, and economic balances for all process units were incorporated in a nonlinear optimization routine for predicting the minimum selling price based on a discounted cash flow rate of return on investment. The optimization utilized a simultaneous-modular approach which was incorporated into the public version of the Aspen flowsheeting package, and used an infeasible path convergence method based on successive quadratic programming procedures. Electrolyte vapour-liquid equilibrium data were estimated by the ’non-random two-liquid’ model. The Lagrangian multipliers of the constraint equations were used to determine the sensitivity of the optimum to key process variables. The method was illustrated by evaluation of two process flowsheets for electrosynthesis of methyl ethyl ketone (MEK) from 1-butene based on pilot-plant performance reported in the patent literature.