In the past few years, the development of inverse design and optimization methods has opened up new possibilities. The adjoint method is of great significance in that context, since it permits high fidelity to flow‐physics at comparatively low computational costs. The present work focuses on adsorbed gas storage systems. Its contribution is the development of an alternative approach to the adjoint contour problem, which ensures that the latter is as well‐posed as the physical problem, itself. This approach proves to be fully consistent with Cacuci's methodology for computing sensitivity derivatives, which enables us to extend their scope. It allows for the evaluation of sensitivities with respect to parameters other than those pertaining to geometry, that is, to those that control the system operation such as average mass flux, convective heat transfer, inlet and external temperature. The main goal of this work is to obtain and validate a basic structure of an optimization loop algorithm (OLA) based on adjoint method, applied to adsorption natural gas storage systems, with pressure and density of adsorption as objective functions.