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Title: FC-PAD Consortium: Fuel Cell Performance and Durability

Abstract

No abstract provided.

Authors:
 [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1238130
Report Number(s):
LA-UR-16-20889
DOE Contract Number:
AC52-06NA25396
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Energy Sciences; Fuel Cell Durability and Performance

Citation Formats

Borup, Rodney L. FC-PAD Consortium: Fuel Cell Performance and Durability. United States: N. p., 2016. Web. doi:10.2172/1238130.
Borup, Rodney L. FC-PAD Consortium: Fuel Cell Performance and Durability. United States. doi:10.2172/1238130.
Borup, Rodney L. Fri . "FC-PAD Consortium: Fuel Cell Performance and Durability". United States. doi:10.2172/1238130. https://www.osti.gov/servlets/purl/1238130.
@article{osti_1238130,
title = {FC-PAD Consortium: Fuel Cell Performance and Durability},
author = {Borup, Rodney L.},
abstractNote = {No abstract provided.},
doi = {10.2172/1238130},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Feb 12 00:00:00 EST 2016},
month = {Fri Feb 12 00:00:00 EST 2016}
}

Technical Report:

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  • No abstract provided.
  • A fuel cell is an electrochemical energy conversion device that produces electricity during the combination of hydrogen and oxygen to produce water. Proton exchange membranes fuel cells are favored for portable applications as well as stationary ones due to their high power density, low operating temperature, and low corrosion of components. In real life operation, the use of pure fuel and oxidant gases results in an impractical system. A more realistic and cost efficient approach is the use of air as an oxidant gas and hydrogen from hydrogen carriers (i.e., ammonia, hydrocarbons, hydrides). However, trace impurities arising from different hydrogenmore » sources and production increases the degradation of the fuel cell. These impurities include carbon monoxide, ammonia, sulfur, hydrocarbons, and halogen compounds. The International Organization for Standardization (ISO) has set maximum limits for trace impurities in the hydrogen stream; however fuel cell data is needed to validate the assumption that at those levels the impurities will cause no degradation. This report summarizes the effect of selected contaminants tested at SRNL at ISO levels. Runs at ISO proposed concentration levels show that model hydrocarbon compound such as tetrahydrofuran can cause serious degradation. However, the degradation is only temporary as when the impurity is removed from the hydrogen stream the performance completely recovers. Other molecules at the ISO concentration levels such as ammonia don't show effects on the fuel cell performance. On the other hand carbon monoxide and perchloroethylene shows major degradation and the system can only be recovered by following recovery procedures.« less
  • The main objectives of this project were to investigate the effect of a series of potential impurities on fuel cell operation and on the particular components of the fuel cell MEA, to propose (where possible) mechanism(s) by which these impurities affected fuel cell performance, and to suggest strategies for minimizing these impurity effects. The negative effect on Pt/C was to decrease hydrogen surface coverage and hydrogen activation at fuel cell conditions. The negative effect on Nafion components was to decrease proton conductivity, primarily by replacing/reacting with the protons on the Bronsted acid sites of the Nafion. Even though already wellmore » known as fuel cell poisons, the effects of CO and NH3 were studied in great detail early on in the project in order to develop methodology for evaluating poisoning effects in general, to help establish reproducibility of results among a number of laboratories in the U.S. investigating impurity effects, and to help establish lower limit standards for impurities during hydrogen production for fuel cell utilization. New methodologies developed included (1) a means to measure hydrogen surface concentration on the Pt catalyst (HDSAP) before and after exposure to impurities, (2) a way to predict conductivity of a Nafion membranes exposed to impurities using a characteristic acid catalyzed reaction (methanol esterification of acetic acid), and, more importantly, (3) application of the latter technique to predict conductivity on Nafion in the catalyst layer of the MEA. H2-D2 exchange was found to be suitable for predicting hydrogen activation of Pt catalysts. The Nafion (ca. 30 wt%) on the Pt/C catalyst resides primarily on the external surface of the C support where it blocks significant numbers of micropores, but only partially blocks the pore openings of the meso- and macro-pores wherein lie the small Pt particles (crystallites). For this reason, even with 30 wt% Nafion on the Pt/C, few Pt sites are blocked and, hence, are accessible for hydrogen activation. Of the impurities studied, CO, NH3, perchloroethylene (also known as tetrachloroethylene), tetrahydrofuran, diborane, and metal cations had significant negative effects on the components in a fuel cell. While CO has no effect on the Nafion, it significantly poisons the Pt catalyst by adsorbing and blocking hydrogen activation. The effect can be reversed with time once the flow of CO is stopped. NH3 has no effect on the Pt catalyst at fuel cell conditions; it poisons the proton sites on Nafion (by forming NH4+ cations), decreasing drastically the proton conductivity of Nafion. This poisoning can slowly be reversed once the flow of NH3 is stopped. Perchloroethylene has a major effect on fuel cell performance. Since it has little/no effect on Nafion conductivity, its poisoning effect is on the Pt catalyst. However, this effect takes place primarily for the Pt catalyst at the cathode, since the presence of oxygen is very important for this poisoning effect. Tetrahydrofuran was shown not to impact Nafion conductivity; however, it does affect fuel cell performance. Therefore, its primary effect is on the Pt catalyst. The effect of THF on fuel cell performance is reversible. Diborane also can significant affect fuel cell performance. This effect is reversible once diborane is removed from the inlet streams. H2O2 is not an impurity usually present in the hydrogen or oxygen streams to a fuel cell. However, it is generated during fuel cell operation. The presence of Fe cations in the Nafion due to system corrosion and/or arising from MEA production act to catalyze the severe degradation of the Nafion by H2O2. Finally, the presence of metal cation impurities (Na+, Ca 2+, Fe3+) in Nafion from MEA preparation or from corrosion significantly impacts its proton conductivity due to replacement of proton sites. This effect is not reversible. Hydrocarbons, such as ethylene, might be expected to affect Pt or Nafion but do not at a typical fuel cell temperature of 80oC. In the presence of large quantities of hydrogen on the anode side, ethylene is converted to ethane which is very nonreactive. More surprisingly, even more reactive hydrocarbons such as formic acid and acetaldehyde do not appear to react enough with the strong Bronsted acid sites on Nafion at such low temperatures to affect Nafion conductivity properties. These results clearly identify a number of impurities which can have a detrimental impact on fuel cell performance, although some are reversible. Obviously, fuel cells exposed to impurities/poisons which are reversible can recover their original performance capabilities once the impurity flow is stopped. Impurities with irreversible effects should be either minimized in the feed streams, if possible, or new catalytic materials or ion conductors will need to be used to minimize their impact.« less
  • This program is focused on the experimental determination of the effects of key hydrogen side impurities on the performance of PEM fuel cells. Experimental data has been leveraged to create mathematical models that predict the performance of PEM fuel cells that are exposed to specific impurity streams. These models are validated through laboratory experimentation and utilized to develop novel technologies for mitigating the effects of contamination on fuel cell performance. Results are publicly disseminated through papers, conference presentations, and other means.
  • The impact of contaminants on fuel cell performance was examined to document air filter specifications (prevention) and devise recovery procedures (maintenance) that are effective at the system level. Eight previously undocumented airborne contaminants were selected for detailed studies and characterization data was used to identify operating conditions that intensifying contamination effects. The use of many and complementary electrochemical, chemical and physical characterization methods and the derivation of several mathematical models supported the formulation of contamination mechanisms and the development of recovery procedures. The complexity of these contamination mechanisms suggests a shift to prevention and generic maintenance measures. Only two ofmore » the selected contaminants led to cell voltage losses after injection was interrupted. Proposed recovery procedures for calcium ions, a component of road de-icers, dessicants, fertilizers and soil conditioners, were either ineffective or partly effective, whereas for bromomethane, a fumigant, the cell voltage was recovered to its initial value before contamination by manipulating and sequencing operating conditions. However, implementation for a fuel cell stack and system remains to be demonstrated. Contamination mechanisms also led to the identification of membrane durability stressors. All 8 selected contaminants promote the formation of hydrogen peroxide, a known agent that can produce radicals that attack the ionomer and membrane molecular structure whereas the dehydrating effect of calcium ions on the ionomer and membrane increases their brittleness and favors the creation of pinholes under mechanical stresses. Data related to acetylene, acetonitrile and calcium ions are emphasized in the report.« less