Mechanisms of proton conductance in polymer electrolyte membranes

被引:314
作者
Eikerling, M
Kornyshev, AA [1 ]
Kuznetsov, AM
Ulstrup, J
Walbran, S
机构
[1] Res Ctr Julich GMBH, Inst Mat & Proc Energy Syst, D-52425 Julich, Germany
[2] Russian Acad Sci, AN Frumkin Electrochem Inst, Moscow 117071, Russia
[3] Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark
关键词
D O I
10.1021/jp003182s
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We provide a phenomenological description of proton conductance in polymer electrolyte membranes, based on contemporary views of proton transfer processes in condensed media and a model for heterogeneous polymer electrolyte membrane structure. The description combines the proton transfer events in a single pore with the total pore-network performance and, thereby, relates structural and kinetic characteristics of the membrane. The theory addresses specific experimentally studied issues such as the effect of the density of proton localization sites (equivalent weight) of the membrane material and the water content of the pores. The effect of the average distance between the sulfonate groups, which changes during membrane swelling, is analyzed in particular, and the factors which determine the temperature dependence of the macroscopic membrane conductance are disclosed. Numerical estimates of the specific membrane conductivity obtained from the theory agree very well with typical experimental data, thereby confirming the appropriateness of the theoretical concepts. Moreover, the versatility of the models offers a useful and transparent frame for combining the analysis of both experimental data and the results of molecular dynamics simulations.
引用
收藏
页码:3646 / 3662
页数:17
相关论文
共 49 条
[1]   The electrical resistivity log as an aid in determining some reservoir characteristics [J].
Archie, GE .
TRANSACTIONS OF THE AMERICAN INSTITUTE OF MINING AND METALLURGICAL ENGINEERS, 1942, 146 :54-61
[2]  
ATKINS PW, 1998, PHYSICAL CHEM, P741
[3]   Characterization of the pore area distribution in porous membranes using transport measurements [J].
Baltus, RE .
JOURNAL OF MEMBRANE SCIENCE, 1997, 123 (02) :165-184
[4]   EFFECTIVE-MEDIUM THEORIES FOR SITE-DISORDERED RESISTANCE NETWORKS [J].
BERNASCONI, J ;
WIESMANN, HJ .
PHYSICAL REVIEW B, 1976, 13 (03) :1131-1139
[5]  
Brack HP, 2000, ACS SYM SER, V744, P174
[6]   CONDUCTANCE OF NAFION-117 MEMBRANES AS A FUNCTION OF TEMPERATURE AND WATER-CONTENT [J].
CAPPADONIA, M ;
ERNING, JW ;
NIAKI, SMS ;
STIMMING, U .
SOLID STATE IONICS, 1995, 77 :65-69
[7]   LOW-TEMPERATURE PROTON TRANSPORT IN CLATHRATES [J].
CAPPADONIA, M ;
KORNYSHEV, AA ;
KRAUSE, S ;
KUZNETSOV, AM ;
STIMMING, U .
JOURNAL OF CHEMICAL PHYSICS, 1994, 101 (09) :7672-7682
[8]  
CHIZMADZHEV YA, 1971, MACROKINETICS PROCES, pCH6
[9]   High-temperature proton conducting membranes based on perfluorinated ionomer membrane-ionic liquid composites [J].
Doyle, M ;
Choi, SK ;
Proulx, G .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2000, 147 (01) :34-37
[10]  
DULLIEN F, 1979, POROUS MEDIA FLUID T, pCH4