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Affordable thin-film composite (TFC) membranes are a potential alternative to more expensive ion exchange membranes in saltwater electrolyzers used for hydrogen gas production. We used a solution-friction transport model to study how the induced potential gradient controls ion transport across the polyamide (PA) active layer and support layers of TFC membranes during electrolysis. The set of parameters was simplified by assigning the same size-related partition and friction coefficients for all salt ions through the membrane active layer. The model was fit to experimental ion transport data from saltwater electrolysis with 600 mM electrolytes at 10 mA cm–2. When the electrolyte concentration and current density were increased, the transport of major charge carriers was successfully predicted by the model. Ion transport calculated using the model only minimally changed when the negative active layer charge density was varied from 0 to 600 mM, indicating active layer charge was not largely responsible for controlling ion crossover during electrolysis. Based on model simulations, a sharp pH gradient was predicted to occur within the supporting layer of the membrane. These results can help guide membrane design and operation conditions in water electrolyzers using TFC membranes. 

Low-cost polyamide thin-film composite membranes are being explored as alternatives to expensive cation exchange membranes for seawater electrolysis. However, chloride transport from seawater to the anode chamber must be reduced to minimize production of chlorine gas. A double-polyamide membrane composite structure was created that reduced chloride transport. Adding five polyamide layers on the back of a conventional polyamide composite membrane reduced chloride ion transport by 53% and did not increase the applied voltage. Decelerated chloride permeation was attributed to enhanced electrostatic and steric repulsion created by the new polyamide layer. Charge was balanced through increased sodium ion transport (52%) from the anolyte to the catholyte rather than a change in water ion transport. As a result, the Nernstian loss arising from the pH difference between the anolyte and catholyte remained relatively constant during electrolysis despite membrane modifications. This lack of a change in pH showed that transport of proton and hydroxide during electrolysis was independent of salt ion transport. Therefore, only sodium ion transport could compensate for the reduction of chloride flux to maintain the set current. Overall, these results prove the feasibility of using double-polyamide structure to control chloride permeation during seawater electrolysis without sacrificing energy consumption.