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The passage of an electrical current through phosphoric acid doped polymer membranes involves parasitic migration of the acid, which imposes a critical issue for long-term operation of the high temperature polymer electrolyte membranes fuel cell (HT-PEMFC). To elucidate the phenomenon, a three-layered membrane is constructed with embedded micro reference electrodes to measure phosphoric acid redistribution in a polybenzimidazole based membrane. Under a constant load, a concentration gradient develops due to the acid migration, which drives the back diffusion of the acid and eventually reaches a steady state between migration and diffusion. The acid gradient is measured as a difference in local ohmic resistances of the anode- and cathode-layer membranes by electrochemical impedance spectroscopy. The phosphoric acid diffusion coefficient through the acid doped membrane is about 10−11 m2 s−1, at least one order of magnitude lower than that of aqueous phosphoric acid solutions. The anion (H2PO4−) transference number is found to range up to 4% depending on current density, temperature and atmospheric humidity of the cell, implying that careful control of the operating parameters is needed in order to suppress the vehicular proton conduction as a degradation mitigation strategy.

Determination of Anion Transference Number and Phosphoric Acid Diffusion Coefficient in High Temperature Polymer Electrolyte Membranes