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The design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e- due to peroxide/radicals scavenging effect of Mn. [Display omitted] • Bi-metallic Fe-Mn-N-C PGM-free catalysts were synthesized. • Highly performed, industrial quality MEAs were fabricated. • Detailed electrochemical fuel cell evaluation was combined with EIS modeling. • The proton conductivity in catalyst layer was improved 5 times vs literature data. [ABSTRACT FROM AUTHOR]

Abstract: This work presents a study of multi-phase flow through the cathode side of a polymer electrolyte membrane fuel cell employing an interdigitated flow field plate. A previously published model has been extended in order to account for phase change kinetics, and a comparison between the interdigitated flow field design and a conventional straight channel design has been conducted. It is found that the parasitic pressure drop in the interdigitated design is in the range of a few thousand Pa and could be reduced to a few hundred Pa by choosing diffusion media with high in-plane permeability. The additional compressor work due to the increased pressure loss will only slightly increase, and this may be offset by operating at lower stoichiometries as the interdigitated design is less mass transfer controlled, which means that the overall efficiency of the interdigitated arrangement will be higher. In the interdigitated design more product water is carried out of the cell in the vapor phase compared to the straight channel design which indicates that liquid water management might be less problematic. This effect also leads to the finding that in the interdigitated design more waste heat is carried out of the cell in the form of latent heat which reduces the load on the coolant. Finally we see that the micro-porous layer might help keep the gas diffusion layer substrate dry due to a potentially higher evaporation rate caused by a combination of the Kelvin effect and a larger specific surface area compared to the diffusion layer substrate. [Copyright &y& Elsevier]

A three-dimensional multiphase mode! that describes the liquid water flux through the porous media and into the gas flow channel of a proton exchange membrane fuel cell (PEMFC) cathode is presented. The mode! is based on the multifluid approach, thus solving one complete set of transport equations for each phase. It is used to investigate the effect of different material parameters on the predicted liquid water saturation in various layers, i.e., catalyst layer (CL), microporous layer (MPL), and gas diffusion layer (GDL). Each layer can be characterized by its porosity, permeability, and contact angle, while the Leverett function was used to describe the capillary pressure vs saturation. The irreducible saturation can be specified for each layer independent!y. An expression for the channel/GDL interface condition was developed, which accounts for the number of drop!ets per unit area at the GDL interface. Describing the different porous media by Leverett equations leads to a jump condition in saturation across each interface. In accordance with previous studies it is found that the MPL remains at a low saturation level, while the CL might become flooded depending on the fraction of hydrophilic pores. Under-the-land compression leads to an increased level of flooding compared to the channel section. [ABSTRACT FROM AUTHOR]

A family of novel carbon materials with intermediate surface area and varying morphology and surface chemistry were used to prepare Pt/C catalysts by two different preparation procedures; a chemical impregnation method and a microwave-assisted polyol method. The catalysts were thoroughly characterized, and their electrochemical performance and stability were investigated with rotating disc electrode (RDE) cyclic voltammetric (CV) measurements. The intermediate-surface-area carbon supports gave catalysts with much greater support stability than a widely used standard catalyst. The novel catalysts had lower electrochemical surface area than the reference, but their specific electrocatalytic activity towards the oxygen-reduction reaction (ORR) was much higher, and some of them also featured higher mass-specific ORR activity than the reference. The series of catalysts prepared by the microwave-assisted polyol method featured smaller Pt nanoparticles and higher activities than those prepared by impregnation. On the other hand, the impregnated catalysts showed better durability of the Pt particles. The most promising catalysts were selected and elaborated in further optimized preparation procedures to obtain quantities sufficient for their use in proton-exchange membrane fuel cells (PEMFCs). [ABSTRACT FROM AUTHOR]

Carbon-based catalyst support and Pt catalysts are commonly used in polymer electrolyte fuel cells (PEFCs). During cell start-up and shutdown processes, carbon support oxidation occurs, which leads to losses of electrochemical performance. In this work, carbon corrosion accelerated stress tests (ASTs) were performed and lifetimes of high surface area carbon (HSAC) and graphitized carbon (GrC) supports were investigated. 1000 AST cycles were conducted on Pt/HSAC while 10000 AST cycles were conducted on Pt/GrC due to different carbon corrosion rates, and both Pt/HSAC and Pt/GrC showed rapid decrease of performance at end of life (EOL). Detailed comparisons of electrochemical characterizations were also conducted between Pt/HSAC and Pt/GrC. Electrochemical surface area (ECSA) loss in different levels was found for both Pt/HSAC and Pt/GrC due to Pt loss, Pt detachment and particles coalescence, which also resulted in reduction of S O 3 − group coverage and more tortuous H + transportation, leading to decreased catalyst layer ionic conductivity. For Pt/HSAC after 1000 AST cycles, more than 2 times higher ECSA loss but with only 50% greater particle size growth and similar Pt loss strongly suggested that a greater Pt detachment occurred on HSAC support during the AST cycles. Apart from that, it was found that after 1000 AST cycles, graphitized carbon support was much more robust compared to HSAC support, and it showed 2 times less ECSA reduction, 2.5 times less catalyst layer ionic conductivity reduction and 4 times less S O 3 − group coverage reduction. Double layer capacitances increased for both carbon supports after AST at their EOLs, as more disordered carbon contacts were formed, which created more contacts between solid and ionic materials. This study shows a possibility of Pt/GrC catalysts to meet the Department of Energy (DOE) target of 5000 AST carbon cycles, as the Pt/GrC cell met the target of ≤ 40% ECSA loss of initial area. • Carbon corrosion tests are performed for two supports for fuel cells. • Graphitized support maintained high surface area after 5000 cycles. • High surface area carbon support layer lost most of its thickness after 1000 cycles. [ABSTRACT FROM AUTHOR]

A new platinum group metal (PGM)-free proton exchange membrane fuel cell (PEMFC) cathode catalyst materials, synthesized using the VariPore™ method by Pajarito Powder, LLC, are characterized for their structure and activity. The physico-chemical analysis of the iron-nitrogen-carbon (Fe-N-C) electrocatalysts show mesoporous carbon material effectively doped with iron and nitrogen. The materials have an average pore size of 7–8 nm and high specific surface area. The Fe-N-C catalysts exhibit good oxygen reduction reaction (ORR) activity in 0.5 M H 2 SO 4 electrolyte with high half-wave potential and sustainable electrochemical stability over 10,000 repeated potential cycles with insignificant losses in their activities. As cathode catalysts in a PEMFC, the Fe-N-C materials deliver remarkably good fuel cell performance at low overpotential approaching that of the commercial Pt catalyst. The high ORR electrocatalytic activity of these Fe-N-C catalysts is credited to the synergy between nitrogen-moieties, specifically pyrrolic-N, pyridinic-N, and graphitic-N, and iron in addition to the high mesoporosity that facilitate an effective reaction path in boosting the electrocatalytic activity and stability. [Display omitted] • State-of-the-art commercial PGM-free catalysts for ORR were characterized and evaluated. • Was shown that active centres are atomically dispersed. • Performance of electrocatalysts was evaluated in industrially manufactured MEA form-factor. • The fuel cell performance is close to the state-of-the-art R&D PGM-free catalysts. [ABSTRACT FROM AUTHOR]

To elucidate the evolution of ionomer-Pt and ionomer-carbon interfaces during life cycle of polymer electrolyte fuel cells (PEFCs), electrodes with high surface area (HSA) and durable carbon supports underwent catalyst and carbon corrosion accelerated stress tests (ASTs) under stoichiometric and sub-stoichiometric gas flow conditions. Electrochemical characterizations, as well as X-ray photoelectron spectroscopy (XPS) were utilized to assess degree of components degradation. Catalyst AST results revealed that Pt nanoparticles dispersed within the micro- and meso-pores and not in contact with ionomer are the main contributor to the 50% electrochemical surface area (ECSA) loss observed after 30k cycles resulting in significant polarization loss, which is much more notable in the case of sub-stoichiometric operating condition. Support AST results for HSA carbon showed severe ionomer degradation and 55% ECSA loss within the first 100 cycles, while cell with durable support exhibited negligible polarization and ECSA decay during the first 2500 cycles attributed to higher ionomer coverage, preservation of proton pathways preventing Pt from detachment. [Display omitted] • Interfaces evolution are evaluated during accelerated stress tests (ASTs) for fuel cells. • Pt that is not in contact with ionomer degrades the most for catalyst AST. • Ionomer degradation is observed for all ASTs. • Graphitized carbon supports mitigate corrosion and Pt loss. [ABSTRACT FROM AUTHOR]