1. |
- Grimler, Henrik
(författare)
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Limiting processes in anion-exchange membrane fuel cells
- 2022
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Fuel cells allow for converting chemical energy stored in hydrogen into electrical energy, with only heat and water as by-products. In a sustainable energy society, hydrogen may play an important role due to its ability to act both as an energy carrier and as a valuable chemical in the process industry. The main remaining obstacles for widely available commercial fuel cells are durability and cost. One way to potentially decrease the cost is to change the fuel cell environment to an alternative chemistry by replacing the proton-exchange membrane (PEM) with an anion-exchange membrane (AEM). This thesis studies the anode reaction, the cathode reaction and water transport in an anion-exchange membrane fuel cell (AEMFC), to investigate where its performance limitations lies in the system. Electrochemical characterisation techniques together with physics-based modelling have been utilised.The results from the study of the anode, shows that the hydrogen reaction proceeds through the Tafel-Volmer pathway, with the Tafel step starting to limit the reaction as the anode overpotential increases. Combining the anode model with a Butler-Volmer expression for the cathode reaction made it possible to model a H2:O2 fuel cell. Comparing the losses from the different processes in the fuel cell shows that the cathode is still the main contributor, but that the anode contribution cannot be neglected when predicting the fuel cell performance. Low ionic conductivity in the electrode was also identified as responsible for part of the overall resistances, leading to uneven current distribution in the catalyst layers and bad utilisation of the catalytic material.Investigating the water transport properties of AEMs showed that not only electroosmotic drag and diffusion, but also an absorption/desorption step between gas phase and membrane phase, are necessary to get a model that can explain the experimental observations. The choice of gas diffusion layers (GDLs) used on the anode and cathode was found to be of similar importance on the water transport as doubling the membrane thickness, showing that not only the membrane is important for water transport. Under most realistic conditions, the risk of local dry-out in a cell was found to be low, as water readily diffuses from the high humidity side of the membrane to the low humidity side.
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2. |
- Acevedo Gomez, Yasna, et al.
(författare)
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Performance Recovery after Contamination with Nitrogen Dioxide in a PEM Fuel Cell
- 2020
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Ingår i: Molecules. - : MDPI. - 1431-5157 .- 1420-3049. ; 25:5
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Tidskriftsartikel (refereegranskat)abstract
- While the market for fuel cell vehicles is increasing, these vehicles will still coexist with combustion engine vehicles on the roads and will be exposed to an environment with significant amounts of contaminants that will decrease the durability of the fuel cell. To investigate different recovery methods, in this study, a PEM fuel cell was contaminated with 100 ppm of NO2 at the cathode side. The possibility to recover the cell performance was studied by using different airflow rates, different current densities, and by subjecting the cell to successive polarization curves. The results show that the successive polarization curves are the best choice for recovery; it took 35 min to reach full recovery of cell performance, compared to 4.5 h of recovery with pure air at 0.5 A cm(-2) and 110 mL min(-1). However, the performance recovery at a current density of 0.2 A cm(-2) and air flow 275 mL min(-1) was done in 66 min, which is also a possible alternative. Additionally, two operation techniques were suggested and compared during 7 h of operation: air recovery and air depletion. The air recovery technique was shown to be a better choice than the air depletion technique.
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3. |
- Benamira, M., et al.
(författare)
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Gadolinia-doped ceria mixed with alkali carbonates for SOFC applications : II - An electrochemical insight
- 2012
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Ingår i: International journal of hydrogen energy. - : Elsevier BV. - 0360-3199 .- 1879-3487. ; 37:24, s. 19371-19379
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Tidskriftsartikel (refereegranskat)abstract
- Composite materials based on gadolinia-doped ceria (GDC) and alkali carbonates (Li2CO3-K2CO3 or Li2CO3-Na2CO3) are potential electrolytes for low temperature solid oxide fuel cell applications (LTSOFC). This paper completes a first one dedicated to the thermal, structural and morphological study of such compounds; it is fully focussed on their electrical/electrochemical properties in different conditions, temperature, composition and gaseous atmosphere (oxidative or reductive). The influence of the gaseous composition on the Arrhenius conductivity plots is evidenced, in particular under hydrogen atmosphere. Finally, electrical conductivity determined by impedance spectroscopy is presented as a function of time to highlight the stability of such composites over 6000 h. First results on single cells showed performance at 600 degrees C of 60 mW cm(-2).
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5. |
- Brown, Rosemary, 1990, et al.
(författare)
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Surface Composition of a Highly Active Pt3Y Alloy Catalyst for Application in Low Temperature Fuel Cells
- 2020
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Ingår i: Fuel Cells. - : Wiley. - 1615-6846 .- 1615-6854. ; 20:4, s. 413-419
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Tidskriftsartikel (refereegranskat)abstract
- Currently, platinum is the most widely used catalyst for low temperature proton exchange membrane fuel cells (PEMFC). However, the kinetics at the cathode are slow, and the price of platinum is high. To improve oxygen reduction reaction (ORR) kinetics at the cathode, platinum can be alloyed with rare earth elements, such as yttrium. We report that Pt3Y has the potential to be over 2 times more active for the ORR compared with Pt inside a real fuel cell. We present detailed photoemission analysis into the nature of the sputtered catalyst surface, using synchrotron radiation photoelectron spectroscopy (SRPES) to examine if surface adsorbates or impurities are present and can be removed. Pretreatment removes most of the yttrium oxide in the surface leaving behind a Pt overlayer which is only a few monolayers thick. Evidence of a substochiometric oxide peak in the Y 3d core level is presented, this oxide extends into the surface even after Ar+ sputter cleaning in-situ. This information will aid the development of new highly active nanocatalysts for employment in real fuel cell electrodes.
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6. |
- Butori, Martina, et al.
(författare)
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The effect of oxygen partial pressure and humidification in proton exchange membrane fuel cells at intermediate temperature (80-120 degrees C)
- 2023
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Ingår i: Journal of Power Sources. - : Elsevier BV. - 0378-7753 .- 1873-2755. ; 563, s. 232803-
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Tidskriftsartikel (refereegranskat)abstract
- The integration of proton exchange membrane fuel cells (PEMFCs) in heavy-duty vehicles would be facilitated if operating temperatures above 100 degrees C were possible. In this work, the effect of temperature in the intermediate range of 80-120 degrees C is investigated for a commercial membrane electrode assembly (MEA) through polarization curves and electrochemical impedance spectroscopy. The importance of oxygen partial pressure on voltage is systematically studied by decoupling it from humidity and temperature. The results show that adequate oper-ation at intermediate temperature is achievable if the oxygen partial pressure is sufficient. Although the cathode kinetics is faster with rising temperatures, the voltage gain is counteracted by the decreasing equilibrium po-tential. At intermediate temperature, the water transport is enhanced, levelling out the relative humidity dif-ference between anode and cathode. However, ionic conductivity in the polymer can become limiting at high currents, due to a smaller relative humidity increase at these temperatures. To conclude, a higher operating temperature does not inherently cause a decrease in obtained current density. Rather, the difficulty to simul-taneously have sufficient oxygen partial pressure and high relative humidity causes limitations within the cathode that to some extent can be solved by pressurizing the cell.
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7. |
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8. |
- Carlson, Annika
(författare)
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Electrochemical properties of alternative polymer electrolytes in fuel cells
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Fuel cells, using hydrogen as energy carrier, allow chemically‑stored energy to be utilized for many applications, including balancing the electrical grid and the propulsion of vehicles. To make the fuel cell technology more accessible and promote a sustainable energy society, this thesis focuses on alternative polymer electrolytes, as they can potentially lead to a lower cost and a more environmentally‑friendly fuel cell. The main subject is anion exchange membrane fuel cells (AEMFCs), for which the importance of gas diffusion electrode morphology and platinum electrode reactions are investigated. Properties of the membrane such as water flux during operation are evaluated. Furthermore, novel polymer electrolytes are studied: variations of poly(phenylene oxide)‑based membranes in AEMFCs; and cellulose‑based membranes in a proton exchange membrane fuel cell (PEMFC). The AEMFC results show that the performance is dependent on the electrode morphology. Electrochemical experiments in a hydrogen/hydrogen cell combined with modelling show that the hydrogen oxidation reaction proceeds through the Tafel‑Volmer reaction pathway on platinum. Application of the model in a hydrogen/oxygen cell shows that the cathode has the slowest reaction rate. During operation, the water flux through the membrane is directed from the anode where water is produced to the cathode where it is consumed. This leads to an increase in water content at both electrodes, which implies that electrode flooding is more likely than dry‑out during operation. The effect of membrane thickness on water flux is shown to be larger than the effect of polymer structure for several different types of poly(phenylene oxide)‑based membranes. The comparison of these polymers also indicates that a high conductivity, for the relative humidity achieved in a fuel cell, promotes increased performance. Finally, the study of cellulose-based membranes in a PEMFC shows that cellulose as a renewable, natural polymer has promising properties, such as stable conductivity for relative humidities above 65 % and a low gas permeability.
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9. |
- Carlson, Annika, et al.
(författare)
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Electrode parameters and operating conditions influencing the performance of anion exchange membrane fuel cells
- 2018
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Ingår i: Electrochimica Acta. - : Elsevier. - 0013-4686 .- 1873-3859. ; 277, s. 151-160
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Tidskriftsartikel (refereegranskat)abstract
- A deeper understanding of porous electrode preparation and performance losses is necessary to advance the anion exchange membrane fuel cell (AEMFC) technology. This study has investigated the performance losses at 50 °C for varied: Tokuyama AS-4 ionomer content in the catalyst layer, Pt/C loading and catalyst layer thickness at the anode and cathode, relative humidity, and anode catalyst. The prepared gas diffusion electrodes in the interval of ionomer-to-Pt/C weight ratio of 0.4–0.8 or 29–44 wt% ionomer content show the highest performance. Varying the loading and catalyst layer thickness simultaneously shows that both the cathode and the anode influence the cell performance. The effects of the two electrodes are shown to vary with current density and this is assumed to be due to non-uniform current distribution throughout the electrodes. Further, lowering the relative humidity at the anode and cathode separately shows small performance losses for both electrodes that could be related to lowered ionomer conductivity. Continued studies are needed to optimize, and understand limitations of, each of the two electrodes to obtain improved cell performance.
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10. |
- Carlson, Annika, et al.
(författare)
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Fuel cell evaluation of anion exchange membranes based on poly(phenylene oxide) with different cationic group placement
- 2020
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Ingår i: Sustainable Energy & Fuels. - : Royal Society of Chemistry. - 2398-4902. ; 4:5, s. 2274-2283
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Tidskriftsartikel (refereegranskat)abstract
- Four novel poly(phenylene oxide)-based anion exchange membranes were investigated for electrochemical performance, ionic conductivity and water transport properties in an operating anion exchange membrane fuel cell (AEMFC), using Pt/C gas diffusion electrodes with Tokuyama ionomer. The poly(phenylene oxide)-membranes have a 1- or 5-carbon alkyl spacer between the backbone and a trimethylalkylammonium (TMA) or piperidinium (Pip) cationic group, and ion-exchange capacities (IECs) between 1.5 and 1.9 mequiv g(-1). The polymer with a 5-carbon alkyl spacer, a TMA cationic group, and a higher IEC showed the highest ion conductivity and performance in the AEMFC. The results also show that introducing a 5-carbon alkyl spacer does not improve performance unless the IEC is increased and that exchanging the TMA with a Pip cationic group results in lower fuel cell performance despite a higher IEC. A discrepancy in ion conductivity between fuel cell and ex situ test was observed for the 5-carbon spacer polymers and is attributed to a higher sensitivity for dehydration. Similar water flux under load, from the anode to the cathode with increased water content at both electrodes, was observed for all membranes and only varied with membrane thickness. The deviation in fuel cell performance observed between the membranes could not be explained by differences in water flux or ionic conduction, suggesting that the electrode-membrane interaction plays a major role. Nevertheless, the study emphasizes that high membrane conductivity (for the lambda-range in a fuel cell) and efficient water transport (obtained by lower membrane thickness) promote higher electrochemical performance.
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