CoChat
Sign Up
Cited by 33Fuel Cells and Related MaterialsAdvancements in Solid Oxide Fuel CellsMembrane-based Ion Separation Techniques

The DOI matches its Crossref record; 4 of the 4 references it cites were found in a registry or an index.

Transport in Proton Exchange Membranes for Fuel Cell Applications—A Systematic Non-Equilibrium Approach

Open access
Rangel-Cárdenas, Angie, Koper, Ger·2017·Materials
DOI 10.3390/ma10060576PMC PMC5552083
Open this paper in CoChat — free accountOpen PDF

Abstract

We hypothesize that the properties of proton-exchange membranes for fuel cell applications cannot be described unambiguously unless interface effects are taken into account. In order to prove this, we first develop a thermodynamically consistent description of the transport properties in the membranes, both for a homogeneous membrane and for a homogeneous membrane with two surface layers in contact with the electrodes or holder material. For each subsystem, homogeneous membrane, and the two surface layers, we limit ourselves to four parameters as the system as a whole is considered to be isothermal. We subsequently analyze the experimental results on some standard membranes that have appeared in the literature and analyze these using the two different descriptions. This analysis yields relatively well-defined values for the homogeneous membrane parameters and estimates for those of the surface layers and hence supports our hypothesis. As demonstrated, the method used here allows for a critical evaluation of the literature values. Moreover, it allows optimization of stacked transport systems such as proton-exchange membrane fuel cell units where interfacial layers, such as that between the catalyst and membrane, are taken into account systematically.

Overview

The claims and statistics of this paper haven’t been checked yet.

Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.

A few free checks a day · papers already verified open instantly · results are public

Integrity signals

Registry

Crossref · 10.3390/ma10060576

Cites

4 of 4 references verified0 citation errors · 0 not checkable

Statistics

Figures

Figure 1 Electrochemical Impedance Spectroscopy: measurement and analysis techniques.
Figure 1 Electrochemical Impedance Spectroscopy: measurement and analysis techniques.CC BY · PubMed Central
Figure 2 Nafion™ 117 conductivity value comparison. Springer et al. at 80 °C, in-plane, 2-probe (●) [30]; Zawodinski et al. at 30 °C, in-plane, 2-probe (○) [24]; Lee et al. at 60 °C, in-plane, 4-probe (▲) [12]; Lee et al. at 60 °C, in-plane, 2-probe (▽) [12]; Alberti et al., through-plane, 2-probe (♦) [25].
Figure 2 Nafion™ 117 conductivity value comparison. Springer et al. at 80 °C, in-plane, 2-probe (●) [30]; Zawodinski et al. at 30 °C, in-plane, 2-probe (○) [24]; Lee et al. at 60 °C, in-plane, 4-probe (▲) [12]; Lee et al. at 60 °C, in-plane, 2-probe (▽) [12]; Alberti et al., through-plane, 2-probe (♦) [25].CC BY · PubMed Central
Figure 3 Effect of geometry: (a) Springer et al. [30] in-plane (●) vs. Alberti et al. [25] through-plane (○); (b) Lee et al. 2-probe (●) vs. 4-probe measurements (○) [12].
Figure 3 Effect of geometry: (a) Springer et al. [30] in-plane (●) vs. Alberti et al. [25] through-plane (○); (b) Lee et al. 2-probe (●) vs. 4-probe measurements (○) [12].CC BY · PubMed Central
Figure 4 Water permeability. Ise, Kreuer at 27 °C (●) [31]; Rivin et al. at 32 °C (◻) [1]; Zhao et al. at 70 °C (◊) [8]; Majztrik et al. at 80 °C (×) [9]; Zawodinski et al. at 30 °C (♦) [23]; Zhao et al. at 70 °C (◐) [8]; Edmondson et al. at room temperature (⧩) [22].
Figure 4 Water permeability. Ise, Kreuer at 27 °C (●) [31]; Rivin et al. at 32 °C (◻) [1]; Zhao et al. at 70 °C (◊) [8]; Majztrik et al. at 80 °C (×) [9]; Zawodinski et al. at 30 °C (♦) [23]; Zhao et al. at 70 °C (◐) [8]; Edmondson et al. at room temperature (⧩) [22].CC BY · PubMed Central
Figure 5 Permeability and Diffusivity measuring techniques.
Figure 5 Permeability and Diffusivity measuring techniques.CC BY · PubMed Central
Figure 6 Hydrogen permeability. Schalenbach at 80 °C (●) [35]; Broka et al. at 80 °C (◻) [38]; Sakai et al. at 80 °C (◻) [32]; Jiang et al. at 80 °C (extrapolated) (○) [34]; Dry membrane (▲) [35]; Wet membrane (△) [35].
Figure 6 Hydrogen permeability. Schalenbach at 80 °C (●) [35]; Broka et al. at 80 °C (◻) [38]; Sakai et al. at 80 °C (◻) [32]; Jiang et al. at 80 °C (extrapolated) (○) [34]; Dry membrane (▲) [35]; Wet membrane (△) [35].CC BY · PubMed Central
Figure 7 Electro-osmotic drag measuring techniques.
Figure 7 Electro-osmotic drag measuring techniques.CC BY · PubMed Central
Figure 8 Electro-osmotic drag data compilation. Ise, Kreuer at 27 °C (◼) [31]; Kreuer et al. at 27 °C (▽) [40]; Springer et al. at 80 °C (○) [30]; Onda et al. at 80 °C (×) [42]; Kreuer et al. at 80 °C (+) [2]; Zawodinski at 30 °C (⧩) [23].
Figure 8 Electro-osmotic drag data compilation. Ise, Kreuer at 27 °C (◼) [31]; Kreuer et al. at 27 °C (▽) [40]; Springer et al. at 80 °C (○) [30]; Onda et al. at 80 °C (×) [42]; Kreuer et al. at 80 °C (+) [2]; Zawodinski at 30 °C (⧩) [23].CC BY · PubMed Central
Figure 9 K-drag—(a) at 30 °C (◻) Electrophoretic NMR [43]; (▼) Volumetric method [23]; (○) Electrolysis cell [42]; (b) at 80 °C (◻) ENMR [40]; (▽) Volumetric [30]; (◻) Electrolysis cell [42].
Figure 9 K-drag—(a) at 30 °C (◻) Electrophoretic NMR [43]; (▼) Volumetric method [23]; (○) Electrolysis cell [42]; (b) at 80 °C (◻) ENMR [40]; (▽) Volumetric [30]; (◻) Electrolysis cell [42].CC BY · PubMed Central
Figure 10 Comparison: measurements where there are mainly bulk contributions against measurements where mainly interfacial effects are present as compared to corrected overall values.
Figure 10 Comparison: measurements where there are mainly bulk contributions against measurements where mainly interfacial effects are present as compared to corrected overall values.CC BY · PubMed Central

Verification

Claims the paper makes

The claims and statistics of this paper haven’t been checked yet.

Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.

A few free checks a day · papers already verified open instantly · results are public

Claims other papers make about this one

Each is checked against this paper’s own text: does it say what the citing paper says it does?

Self-check

Percentages, sums and reported differences re-computed from the paper’s own numbers.

The self-check needs the paper’s full text.

Citations

Cites

Research works printed but not linked: 40

  1. Rivin, 2001, Solubility and transport behavior of water and alcohols in Nafion™, Polymer, 42, 623, 10.1016/S0032-3861(00)00350-5 · DOI
  2. Kjelstrup, S., and Bedeaux, D. (2008). Non-Equilibrium Thermodynamics of Heterogeneous Systems, World Scientific. · DOI
  3. Onsager, 1931, Reciprocal relations in irreversible processes, I. Phys. Rev., 37, 405, 10.1103/PhysRev.37.405 · DOI
  4. Kjelstrup, S., Bedeaux, D., Johannessen, E., and Gross, J. (2010). Non-Equilibrium Thermodynamics for Engineers, World Scientific Publishing Co. Inc. · DOI
  5. Fuller, 1992, Experimental determination of the transport number of water in Nafion 117 membrane, J. Electrochem. Soc., 139, 1332, 10.1149/1.2069407 · DOI · Paper page
  6. Cooper, 2009, Progress toward accurate through-plane membrane resistance and conductivity measurement, ECS Trans., 25, 995, 10.1149/1.3210653 · DOI
  7. Zhao, 2011, Diffusion and interfacial transport of water in Nafion, J. Phys. Chem. B, 115, 2717, 10.1021/jp1112125 · DOI
  8. Majsztrik, 2007, Water sorption, desorption and transport in Nafion membranes, J. Membr. Sci., 301, 93, 10.1016/j.memsci.2007.06.022 · DOI · Paper page
  9. Cahan, 1993, AC impedance investigations of proton conduction in Nafion™, J. Electrochem. Soc., 140, L185, 10.1149/1.2221160 · DOI
  10. Lee, 2005, Importance of proton conductivity measurement in polymer electrolyte membrane for fuel cell application, Ind. Eng. Chem. Res., 44, 7617, 10.1021/ie0501172 · DOI
  11. Xie, 2006, Discrepancies in the measurement of ionic conductivity of PEMs using two-and four-probe AC impedance spectroscopy, J. Electrochem. Soc., 153, E173, 10.1149/1.2258091 · DOI
  12. Kondepudi, D., and Prigogine, I. (2014). Modern Thermodynamics: From Heat Engines to Dissipative Structures, John Wiley & Sons. · DOI
  13. Newman, J., and Thomas-Alyea, K.E. (2012). Electrochemical Systems, John Wiley & Sons.
  14. Ito, 2011, Properties of Nafion membranes under PEM water electrolysis conditions, Int. J. Hydrogen Energy, 36, 10527, 10.1016/j.ijhydene.2011.05.127 · DOI
  15. Wu, 2011, Differences in water sorption and proton conductivity between Nafion and SPEEK, J. Polym. Sci. B Polym. Phys., 49, 1437, 10.1002/polb.22326 · DOI
  16. Kornyshev, A., Kuznetsov, A.M., Spohr, A., and Ulstrup, J. (2003). Kinetics of Proton Transport in Water, ACS Publications. · DOI
  17. Choe, 2009, Nature of proton dynamics in a polymer electrolyte membrane, nafion: A first-principles molecular dynamics study, Phys. Chem. Chem. Phys., 11, 3892, 10.1039/b819535h · DOI
  18. Edmondson, 2002, Free volume and percolation in S-SEBS and fluorocarbon proton conducting membranes, Solid State Ion., 152, 355, 10.1016/S0167-2738(02)00336-3 · DOI
  19. Zawodzinski, 1994, Water-uptake by and transport through Nafion membranes, J. Electrochem. Soc., 140, 1041, 10.1149/1.2056194 · DOI · Paper page
  20. Alberti, 2001, Polymeric proton conducting membranes for medium temperature fuel cells (110–160 C), J. Membr. Sci., 185, 73, 10.1016/S0376-7388(00)00635-9 · DOI
  21. Edmondson, 2000, Complex impedance studies of proton-conducting membranes, Solid State Ion., 135, 419, 10.1016/S0167-2738(00)00520-8 · DOI
  22. Fontanella, 1996, High-pressure electrical conductivity and NMR studies in variable equivalent weight NAFION membranes, Macromolecules, 29, 4944, 10.1021/ma9600926 · DOI
  23. Kopitzke, 2000, Conductivity and water uptake of aromatic-based proton exchange membrane electrolytes, J. Electrochem. Soc., 147, 1677, 10.1149/1.1393417 · DOI
  24. Navessin, 2005, Influence of membrane ion exchange capacity on the catalyst layer performance in an operating PEM fuel cell, J. Electrochem. Soc., 152, A796, 10.1149/1.1864432 · DOI
  25. Springer, 1991, Polymer electrolyte fuel cell model, J. Electrochem. Soc., 138, 2334, 10.1149/1.2085971 · DOI · Paper page
  26. Sakai, 1986, Gas diffusion in the dried and hydrated Nafions, J. Electrochem. Soc., 133, 88, 10.1149/1.2108551 · DOI
  27. Sakai, 1985, Gas permeation properties of solid polymer electrolyte (SPE) membranes, J. Electrochem. Soc., 132, 1328, 10.1149/1.2114111 · DOI
  28. Jiang, 2004, Investigations of fuel cell reactions at the composite microelectrode| solid polymer electrolyte interface. I. Hydrogen oxidation at the nanostructured Pt|Nafion® membrane interface, J. Electroanal. Chem., 567, 123, 10.1016/j.jelechem.2003.12.018 · DOI
  29. Schalenbach, 2015, Gas Permeation through Nafion. Part 1: Measurements, J. Phys. Chem. C, 119, 25145, 10.1021/acs.jpcc.5b04155 · DOI
  30. Oszcipok, 2002, The compression of hydrogen in an electrochemical cell based on a PE fuel cell design, J. Power Sources, 105, 208, 10.1016/S0378-7753(01)00941-7 · DOI
  31. Felice, 2010, Nafion−montmorillonite nanocomposite membrane for the effective reduction of fuel crossover, Ind. Eng. Chem. Res., 49, 1514, 10.1021/ie901600a · DOI
  32. Broka, 1997, Oxygen and hydrogen permeation properties and water uptake of Nafion® 117 membrane and recast film for PEM fuel cell, J. Appl. Electrochem., 27, 117, 10.1023/A:1018469520562 · DOI
  33. Ye, 2007, Measurement of Water Transport Properties Through Membrane-Electrode Assemblies I. Membranes, J. Electrochem. Soc., 154, B676, 10.1149/1.2737379 · DOI · Paper page
  34. Kreuer, 2001, On the development of proton conducting polymer membranes for hydrogen and methanol fuel cells, J. Membr. Sci., 185, 29, 10.1016/S0376-7388(00)00632-3 · DOI · Paper page
  35. Marangio, 2009, Direct High Pressure Hydrogen Production: A Laboratory Scale PEM Electrolyser Prototype, ECS Trans., 17, 555, 10.1149/1.3142786 · DOI
  36. Onda, 2002, Performance analysis of polymer-electrolyte water electrolysis cell at a small-unit test cell and performance prediction of large stacked cell, J. Electrochem. Soc., 149, A1069, 10.1149/1.1492287 · DOI
  37. Ise, 1999, Electroosmotic drag in polymer electrolyte membranes: An electrophoretic NMR study, Solid State Ion., 125, 213, 10.1016/S0167-2738(99)00178-2 · DOI · Paper page
  38. Siroma, 2002, Proton conductivity along interface in thin cast film of Nafion®, Electrochem. Commun., 4, 143, 10.1016/S1388-2481(01)00290-9 · DOI
  39. Eastman, 2012, Effect of confinement on structure, water solubility, and water transport in Nafion thin films, Macromolecules, 45, 7920, 10.1021/ma301289v · DOI
  40. Zhang, 2014, Thickness-dependent structural and transport behaviors in the platinum–Nafion interface: A molecular dynamics investigation, RSC Adv., 4, 44214, 10.1039/C4RA05523C · DOI

Cited by

Sorted by citations

See all 33

Metadata

Authors
Rangel-Cárdenas, A., & Koper, G.
Affiliations
Delft University of Technology (NL)
Corresponding author
Koper, Ger
ORCID
Venue
Materials
Publisher
MDPI AG
Published
2017-05-25
Volume
10
Issue
6
Pages
576
ISSN
1996-1944 (ISSN-L)
DOI
10.3390/ma10060576
PMC
PMC5552083
OpenAlex
W2618099852
Cited by
33
References
4
Citations by year
2026: 1 · 2025: 3 · 2024: 2 · 2023: 5 · 2022: 3 · 2021: 5 · 2020: 7 · 2019: 1 · 2018: 5 · 2017: 1
FWCI
1.59
Type
journal article
Language
en
Open access
Licence
Locations
  • Materials (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Topics
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
  • Physical Sciences › Materials Science › Materials Chemistry › Advancements in Solid Oxide Fuel Cells
  • Physical Sciences › Chemical Engineering › Filtration and Separation › Membrane-based Ion Separation Techniques
Keywords
proton exchange membranes, fuel cell membranes, membrane transport properties, interface effects, surface layer, thermodynamic consistency, nonequilibrium transport, membrane parameters

About these checks

Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.

Statistics and arithmetic are recomputed, not judged.

Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.

What counts as a claim ›How we measure confidence ›How we check this ›

Are you an author, or do you see a problem with this page? Request a review