1H Solid-State NMR Investigation of Structure and Dynamics of Anhydrous Proton Conducting Triazole-Functionalized Siloxane Polymers

被引:50
作者
Akbey, Uemit [1 ]
Granados-Focil, Sergio [2 ]
Coughlin, E. Bryan [3 ]
Graf, Robert [1 ]
Spiess, Hans Wolfgang [1 ]
机构
[1] Max Planck Inst Polymer Res, D-55128 Mainz, Germany
[2] Clark Univ, Carlson Sch Chem, Worcester, MA 01601 USA
[3] Univ Massachusetts, Dept Polymer Sci & Engn, Amherst, MA 01003 USA
关键词
FUEL-CELLS; MOLECULAR-DYNAMICS; CHEMICAL-SHIFTS; HYDROGEN-BONDS; MEMBRANES; ACID; SPECTROSCOPY; ELECTROLYTE; TRANSPORT; EXCHANGE;
D O I
10.1021/jp9030909
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
H-1 MAS solid-state NMR methods are applied to elucidate the conduction mechanism of an anhydrous proton conducting triazole-functionalized polysiloxane. At temperatures below T= 260 K, hydrogen bonding between neighboring heterocycles is observed and a dimer formation can be excluded. From the temperature dependence of H-1 MAS NMR spectra, different dynamic processes of the triazole ring contributing to the proton conduction process are qualitatively and quantitatively analyzed and detailed insight into the conduction mechanism and temperature-dependent structural changes is obtained. Although the dynamics processes oil the molecular level are qualitatively in good agreement with the findings from macroscopic conductivity measurements, temperature-dependent factors oil mesoscopic scales beyond the local molecular mobility influence the macroscopic Conductivity and hamper quantitative interpretation.
引用
收藏
页码:9151 / 9160
页数:10
相关论文
共 39 条
[1]   Solid-State NMR Investigations of Anhydrous Proton-Conducting Acid-Base Poly(acrylic acid)-Poly(4-vinyl pyridine) Polymer Blend System: A Study of Hydrogen Bonding and Proton Conduction [J].
Akbey, Uemit ;
Graf, Robert ;
Peng, Yuan G. ;
Chu, Peter P. ;
Spiess, Hans W. .
JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS, 2009, 47 (02) :138-155
[2]   FORMATION OF GLASSES FROM LIQUIDS AND BIOPOLYMERS [J].
ANGELL, CA .
SCIENCE, 1995, 267 (5206) :1924-1935
[3]  
[Anonymous], 1983, 1H NUCL MAGNETIC RES
[4]   Solid state 15N NMR and theoretical studies of primary and secondary geometric H/D isotope effects on low-barrier NHN-hydrogen bonds [J].
Benedict, H ;
Limbach, HH ;
Wehlan, M ;
Fehlhammer, WP ;
Golubev, NS ;
Janoschek, R .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (12) :2939-2950
[5]   HETERONUCLEAR DECOUPLING IN ROTATING SOLIDS [J].
BENNETT, AE ;
RIENSTRA, CM ;
AUGER, M ;
LAKSHMI, KV ;
GRIFFIN, RG .
JOURNAL OF CHEMICAL PHYSICS, 1995, 103 (16) :6951-6958
[6]   CORRELATIONS BETWEEN PROTON CHEMICAL-SHIFT TENSORS, DEUTERIUM QUADRUPOLE COUPLINGS, AND BOND DISTANCES FOR HYDROGEN-BONDS IN SOLIDS [J].
BERGLUND, B ;
VAUGHAN, RW .
JOURNAL OF CHEMICAL PHYSICS, 1980, 73 (05) :2037-2043
[7]   TEMPERATURE-DEPENDENCE OF PB-207 MAS SPECTRA OF SOLID LEAD NITRATE - AN ACCURATE, SENSITIVE THERMOMETER FOR VARIABLE-TEMPERATURE MAS [J].
BIELECKI, A ;
BURUM, DP .
JOURNAL OF MAGNETIC RESONANCE SERIES A, 1995, 116 (02) :215-220
[8]   Advanced solid-state NMR methods for the elucidation of structure and dynamics of molecular, macromolecular, and supramolecular systems [J].
Brown, SP ;
Spiess, HW .
CHEMICAL REVIEWS, 2001, 101 (12) :4125-4155
[9]   Probing proton-proton proximities in the solid state [J].
Brown, Steven P. .
PROGRESS IN NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY, 2007, 50 (04) :199-251
[10]   Materials science - Supramolecular polymers [J].
de Greef, Tom F. A. ;
Meijer, E. W. .
NATURE, 2008, 453 (7192) :171-173