Temperature-Dependent Transport Properties of a Redox-Active Ionic Liquid with a Viologen Group

被引:22
作者
Bodappa, Nataraju [1 ]
Broekmann, Peter [1 ]
Fu, Yong-Chun [1 ]
Furrer, Julien [1 ]
Furue, Yutaro [2 ]
Sagara, Takamasa [2 ]
Siegenthaler, Hans [1 ]
Tahara, Hironobu [2 ]
Vesztergom, Soma [1 ,3 ]
Zick, Klaus [4 ]
Wandlowski, Thomas [1 ]
机构
[1] Univ Bern, Dept Chem & Biochem, CH-3012 Bern, Switzerland
[2] Nagasaki Univ, Grad Sch Engn, J-8528521 Nagasaki, Japan
[3] Eotvos Lorand Univ, Dept Phys Chem, H-1117 Budapest, Hungary
[4] Bruker BioSpin GmbH, D-76287 Rheinstetten, Germany
基金
瑞士国家科学基金会;
关键词
PHYSICOCHEMICAL PROPERTIES; CORRELATION-COEFFICIENTS; ELECTRON-TRANSPORT; VISCOSITY; DIFFUSION; ELECTROCHEMISTRY; CONDUCTIVITY; ECHO; FILM;
D O I
10.1021/jp509931p
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
A redox-active ionic liquid (IL), 1-butyl-1'-heptyl-4,4'-bipyridinium bis(trifluoromethanesulfonyl)imide, has been synthesized and its transport processes were investigated. The conductivity and viscosity of the IL, as well as the diffusion coefficients of its components were studied over a 50 degrees C wide temperature range: for the diffusivity studies, both the pulsed-gradient spinecho (PGSE)NMR technique and voltammetric measurements have been applied. The measured data are presented in the paper and are compared to each other. It was found that the diffusion coefficients determined by means of NMR and chronoamperometry measurements are, within the range of experimental error, equaland they are (in accordance with other ionic liquid studies) higher than what the conductivity or viscosity measurements indicate. The results are interpreted in the light of the existing theories. The measured diffusion coefficients and bulk conductivities can be well interrelated based on the ionicity concept (that is, by treating the ionic liquid as a weak electrolyte). In agreement with the empirical Walden rule, a direct comparison between the measured conductivities and viscosities is also possible, for which a hole conduction model is utilized. Based on the fact that both the electrochemical and the NMR measurements yield practically the same diffusion coefficients in the system, there is no evidence that interpretations based in other redox-active IL systems on homogeneous electron transfer apply to the system studied here.
引用
收藏
页码:1067 / 1077
页数:11
相关论文
共 64 条
[1]   Model for the conductivity of ionic liquids based on an infinite dilution of holes [J].
Abbott, AP .
CHEMPHYSCHEM, 2005, 6 (12) :2502-2505
[2]   Application of hole theory to the viscosity of ionic and molecular liquids [J].
Abbott, AP .
CHEMPHYSCHEM, 2004, 5 (08) :1242-1246
[3]   Redox ionic liquid phases: Ferrocenated imidazoliums [J].
Balasubramanian, Ramjee ;
Wang, Wei ;
Murray, Royce W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (31) :9994-9995
[4]  
Bard A.J., 2001, ELECTROCHEMICAL METH, V2nd, P172
[5]   Low viscosity highly conductive ionic liquid blends for redox active electrolytes in efficient dye-sensitized solar cells [J].
Bidikoudi, Maria ;
Zubeir, Lawien F. ;
Falaras, Polycarpos .
JOURNAL OF MATERIALS CHEMISTRY A, 2014, 2 (37) :15326-15336
[6]   ELECTROCHEMISTRY OF THE VIOLOGENS [J].
BIRD, CL ;
KUHN, AT .
CHEMICAL SOCIETY REVIEWS, 1981, 10 (01) :49-82
[7]   Hydrophobic, highly conductive ambient-temperature molten salts [J].
Bonhote, P ;
Dias, AP ;
Papageorgiou, N ;
Kalyanasundaram, K ;
Gratzel, M .
INORGANIC CHEMISTRY, 1996, 35 (05) :1168-1178
[8]   In situ STM investigation of gold reconstruction and of silicon electrodeposition on Au(111) in the room temperature ionic liquid 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide [J].
Borisenko, N ;
El Abedin, SZ ;
Endres, F .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (12) :6250-6256
[9]   Organic layers at metal/electrolyte interfaces: molecular structure and reactivity of viologen monolayers [J].
Breuer, Stephan ;
Pham, Duc T. ;
Huemann, Sascha ;
Gentz, Knud ;
Zoerlein, Caroline ;
Hunger, Ralf ;
Wandelt, Klaus ;
Broekmann, Peter .
NEW JOURNAL OF PHYSICS, 2008, 10
[10]   OHMIC POTENTIAL DROP AT ELECTRODES EXHIBITING STEADY-STATE DIFFUSION CURRENTS [J].
BRUCKENSTEIN, S .
ANALYTICAL CHEMISTRY, 1987, 59 (17) :2098-2101