Abstract

In striving for carbon neutrality, hydrogen energy serves as a sustainable solution, and the iodine–sulfur (IS) cycle stands out as the most promising method for hydrogen production. The separation and purification of HI from the HIx (HI-I2-H2O) mixture holds significant research value, as they constitute the crucial aspect of the iodine–sulfur cycle in hydrogen production. Due to the azeotropic behavior of HI and H2O, the HIx system poses a considerable challenge. In this research, a technique for purifying HI via pressure-swing distillation was developed, exploiting the changes in azeotropic points under varying pressure conditions. The most effective method for HI purification was determined to be a three-column pressure-swing distillation configuration, as revealed by Aspen Plus phase diagrams and process topology mapping. It yielded H2O and I2 at the top of the first column, I2 at the bottom of the second column, and HI at the top of the third column with an HI recovery rate of 97 %. By analyzing the Bunsen reaction kinetics of the core reaction in the IS system, a comprehensive method for evaluating the separation and reaction coupling quality network of HIx cycle system using Bunsen-factor (B-factor) was proposed. The B-factor elucidates the correlation between the Bunsen reaction rate and the concentrations of [H+], [I-], [I3-], as well as the pH level. A comprehensive analysis of the B-factor was conducted for the pressure-swing distillation topologies of the HIx system, and the results were contrasted with those of alternative separation processes. The findings indicated that the three-column pressure-swing distallation is the most suitable option for both separation and reaction quality in a recycled network. The total energy consumption of the newly designed HIx three-column process is 352 MJ/kmol, rendering it more economical and beneficial than other processes. This study presents a pressure-swing distillation method for HI separation and purification, which is broadly applicable in IS cycles and aids in achieving large-scale production of green H2. This method enables the achievement of the dual-carbon objective, which seeks to mitigate carbon emissions while safeguarding the environment.