The economic viability of low temperature fuel cells as clean energy devices is enhanced by the development of inexpensive oxygen reduction reaction catalysts. Heat treated iron and nitrogen containing carbon based materials (Fe–N/C) have shown potential to replace expensive precious metals. Although significant improvements have recently been made, their activity and durability is still unsatisfactory. The further development and a rational design of these materials has stalled due to the lack of an in situ methodology to easily probe and quantify the active site. Here we demonstrate a protocol that allows the quantification of active centres, which operate under acidic conditions, by means of nitrite adsorption followed by reductive stripping, and show direct correlation to the catalytic activity. The method is demonstrated for two differently prepared materials. This approach may allow researchers to easily assess the active site density and turnover frequency of Fe–N/C catalysts.

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Although major progress has recently been achieved through ex situ methods, there is still a lack of understanding of the behavior of the active center in non-precious metal Fe-N/C catalysts under operating conditions. Utilizing nitrite, nitric oxide, and hydroxylamine as molecular probes, we show that the active site for the oxygen reduction reaction (ORR) is different under acidic and alkaline conditions. An in-depth investigation of the ORR in acid reveals a behavior which is similar to that of iron macrocyclic complexes and suggests a contribution of the metal center in the catalytic cycle. We also show that this catalyst is highly active toward nitrite and nitric oxide electroreduction under various pH values with ammonia as a significant byproduct. This study offers fundamental insight into the chemical behavior of the active site and demonstrates a possible use of these materials for nitrite and nitric oxide sensing applications or environmental nitrite destruction.

A pyrolysed carbon–nitrogen based oxygen reduction catalyst is unaffected by a wide range of poisons, which deactivate platinum. The catalyst may allow important devices (fuel cells, metal air batteries, sensors, etc) to operate in “dirty” environments.

30.04.15 KB. Ok to add published ao pape

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Recent experimental data on a fuel cell-like system revealed insights on the fluid flow in both free and porous media. A computational model is used to investigate the momentum and species transport in such system, solved using the finite elements method. The model consists of a stationary, isothermal, diluted species transport in free and porous media flow. The momentum transport is treated using different formulations, namely Stokes-Darcy, Darcy-Brinkman, and a hybrid StokesBrinkman formulations. The species transport is given by the advection equation for a reactant diluted in air. The formulations are compared to each other and to the available experimental data, where it is concluded that the Darcy-Brinkman formulation reproduces the data appropriately. The validated model is used to investigate the contribution of convection in reactant transport in porous media of fuel cells. Convective transport provides a major contribution to reactant distribution in the so-called diffusion media. For a serpentine channel and flow with Re = 260 to 590, convection accounts for 29 to 58% of total reactant transport to the catalyst