Oxidative Degradation of Polybenzimidazole Membranes as Electrolytes for High Temperature Proton Exchange Membrane Fuel Cells

被引:94
作者
Liao, J. H. [1 ,2 ]
Li, Q. F. [1 ]
Rudbeck, H. C. [3 ]
Jensen, J. O. [1 ]
Chromik, A. [4 ]
Bjerrum, N. J. [1 ]
Kerres, J. [4 ]
Xing, W. [2 ]
机构
[1] Tech Univ Denmark, Dept Chem, Energy & Mat Sci Grp, DK-2800 Lyngby, Denmark
[2] Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Jilin, Peoples R China
[3] Danish Power Syst ApS, DK-2920 Charlottenlund, Denmark
[4] Univ Stuttgart, Inst Chem Proc Engn, D-70199 Stuttgart, Germany
关键词
Fuel Cells; Oxidative Degradation; Phosphoric Acid; Polybenzimidazole (PBI); Proton Exchange Membrane; ACID DOPED POLYBENZIMIDAZOLE; PBI; PEMFC; CONDUCTIVITY; PERFORMANCE; POLYETHERS; MODE; MEAS;
D O I
10.1002/fuce.201000146
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
Polybenzimidazole membranes imbibed with acid are emerging as a suitable electrolyte material for high-temperature polymer electrolyte fuel cells. The oxidative stability of polybenzimidazole has been identified as an important issue for the long-term durability of such cells. In this paper the oxidative degradation of the polymer membrane was studied under the Fenton test conditions by the weight loss, intrinsic viscosity, size exclusion chromatography, scanning electron microscopy and Fourier transform infrared spectroscopy. During the Fenton test, significant weight losses depending on the initial molecular weight of the polymer were observed. At the same time, viscosity and SEC measurements revealed a steady decrease in molecular weight. The degradation of acid doped PBI membranes under Fenton test conditions is proposed to start by the attack of hydroxyl radicals at the carbon atom linking imidazole ring and benzenoid ring, which may eventually lead to the imidazole ring opening and formation of small molecules and terminal groups for further oxidation by an endpoint oxidation.
引用
收藏
页码:745 / 755
页数:11
相关论文
共 41 条
[1]  
Buckley A.S., 1987, ENCY POLYM SCI ENG, V11, P572
[2]   Chemical oxidative degradation of Polybenzimidazole in simulated environment of fuel cells [J].
Chang, Zhihong ;
Pu, Hongting ;
Wan, Decheng ;
Liu, Lu ;
Yuan, Junjie ;
Yang, Zhenglong .
POLYMER DEGRADATION AND STABILITY, 2009, 94 (08) :1206-1212
[3]  
Choe EW, 1985, United States Patent, Patent No. [4,535,144, 4535144]
[4]   Proton conducting membranes based on blends of PBI with aromatic polyethers containing pyridine units [J].
Daletou, MK ;
Gourdoupi, N ;
Kallitsis, JK .
JOURNAL OF MEMBRANE SCIENCE, 2005, 252 (1-2) :115-122
[5]   Comparison of the Sulfur Poisoning of PBI and Nafion PEMFC Cathodes [J].
Garsany, Yannick ;
Gould, Benjamin D. ;
Baturina, Olga A. ;
Swider-Lyons, Karen E. .
ELECTROCHEMICAL AND SOLID STATE LETTERS, 2009, 12 (09) :B138-B140
[6]   WEAK-LINK VERSUS ACTIVE CARBON DEGRADATION ROUTES IN OXIDATION OF AROMATIC HETEROCYCLIC SYSTEMS [J].
GAUDIANA, RA ;
CONLEY, RT .
JOURNAL OF POLYMER SCIENCE PART B-POLYMER LETTERS, 1969, 7 (11PB) :793-&
[7]   Investigation of the conduction properties of phosphoric and sulfuric acid doped polybenzimidazole [J].
Glipa, X ;
Bonnet, B ;
Mula, B ;
Jones, DJ ;
Rozière, J .
JOURNAL OF MATERIALS CHEMISTRY, 1999, 9 (12) :3045-3049
[8]   Proton conductivity of phosphoric acid doped polybenzimidazole and its composites with inorganic proton conductors [J].
He, RH ;
Li, QF ;
Xiao, G ;
Bjerrum, NJ .
JOURNAL OF MEMBRANE SCIENCE, 2003, 226 (1-2) :169-184
[9]   Physicochemical properties of phosphoric acid doped polybenzimidazole membranes for fuel cells [J].
He, Ronghuan ;
Li, Qingfeng ;
Bach, Anders ;
Jensen, Jens Oluf ;
Bjerrum, Niels J. .
JOURNAL OF MEMBRANE SCIENCE, 2006, 277 (1-2) :38-45
[10]   EPR investigation of HO. radical initiated degradation reactions of sulfonated aromatics as model compounds for fuel cell proton conducting membranes [J].
Hübner, G ;
Roduner, E .
JOURNAL OF MATERIALS CHEMISTRY, 1999, 9 (02) :409-418