Component durability of polymer-electrolyte membrane (PEM) fuel cells can be improved by adding cerium cations, which serve to scavenge harmful free radicals and selectively decompose hydrogen peroxide, which are formed during the oxidation reduction reaction (ORR). We have investigated the change in distribution of cerium cations in a hydrogen fuel cell as a function of operating time, considering both cerium containing membranes (commercial XL by DuPont) as well as fuel cells with CeO 2 in the cathode catalyst layer. Our results show cerium cations are very mobile in Nafion, and migrate into both the anode and cathode catalyst layers.
CeOx is an excellent free radical scavenger to improve polymer electrolyte membrane durability. However, this metal oxide will dissolve during accelerated stress testing (AST), with the resulting cations transporting to the cathode catalyst layer (CCL) leading to performance reduction/degradation of the PEMFC. Controlling the rate of CeOx dissolution is therefore of great importance, as it may be possible to maintain sufficient Ce cations for free radical scavenging while minimizing the impact of these cations on the CCL. Here the effect of CeOx crystallite size on CeOx dissolution was investigated. Three CeOx additives were prepared having crystallite sizes of 6, 13, or 25 nm. An ex-situ method was used to evaluate the chemical stability of these three CeOx samples, as well as one commercially available CeOx. It was determined that surface area, rather than crystallite size, is the best predictor of chemical stability. In-situ membrane electrode assembly AST cycling was then performed, demonstrating that when low loadings of CeOx (0.006 mg/cm 2 ) are used, the ex-situ method correctly predicts trends in end of life (EOL) performance. Finally, it is shown that increasing the anode RH during AST cycling leads to significantly higher EOL performance losses. Fuel cells are electrochemical devices capable of efficiently converting chemical energy into electrical energy while producing very little pollutants (e.g. NO x , SO x , particulates).1 Due to their higher efficiency and cleaner operation vs. conventional internal combustion engines, fuel cells have become highly promising candidates for clean power generation. Much like a battery, PEMFCs contain an anode, a cathode and an electrolyte. The electrolyte dictates the required operating conditions of the fuel cell (temperature, pH, etc.), and thus fuel cells are classified according to the electrolyte that they employ. Currently, one of the most promising candidates for stationary, mobile, and automotive applications is the proton exchange membrane fuel cell (PEMFC), which utilizes a perfluorinated sulfonic acid (PFSA) polymer membrane (typically Nafion). These membranes must be humidified with liquid water in order for facile proton conduction to occur, and thus PEMFCs typically operate at relatively low temperatures (60-85• C). While PFSA membranes are capable of achieving high proton conductivities (∼10 S/m), they suffer from several modes of degradation during normal operating conditions. 2 Of particular concern are the highly reactive free radicals (OH . , OOH . , H . ) that are formed from the decomposition of H 2 O 2 (an intermediate in the oxygen reduction reaction (ORR)) within the membrane.3-5 While H 2 O 2 alone is not particularly damaging, the presence of even trace amounts of Fenton's catalyst (e.g. Fe 2+ /Fe 3+ ) greatly accelerates the decomposition of H 2 O 2 into aggressive free radicals.6-8 These free radicals are known to attack PFSA membranes through an "unzipping" mechanism in which decomposition is initiated at one end of a PFSA unit and con...
Electrochemical experimentation and modeling indicates that impurities degrade fuel cell performance by a variety of mechanisms. Electrokinetics may be inhibited by catalytic site poisoning by sulfur compounds and CO and by decreased local proton activity and mobility caused by the presence of foreign salt cations or ammonia. Cation impurity profiles vary with current density, valence and may change local conductivity and water concentrations in the ionomer. Nitrogen oxide and ammonia species may be electrochemically active under fuel cell operating conditions. The primary impurity removal mechanisms are electrooxidation and water fluxes through the fuel cell.
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