A new force field model for the simulation of transport properties of imidazolium-based ionic liquids

被引:181
作者
Chaban, Vitaly V. [1 ]
Voroshylova, Iuliia V. [2 ]
Kalugin, Oleg N. [2 ]
机构
[1] Univ Rochester, Dept Chem, Rochester, NY 14642 USA
[2] Kharkov Natl Univ, Fac Chem, UA-61077 Kharkov, Ukraine
关键词
MOLECULAR-DYNAMICS SIMULATION; TEMPERATURE-DEPENDENCE; ATOMISTIC SIMULATION; ELECTRICAL-CONDUCTIVITY; DIFFUSION-COEFFICIENTS; VISCOSITY; DENSITY; CATION; ANION; WATER;
D O I
10.1039/c0cp02778b
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 new, non-polarizable force field model (FFM) for imidazolium-based, room-temperature ionic liquids (RTILs), 1-ethyl-3-methyl-imidazolium tetrafluoroborate and 1-butyl-3-methyl-imidazolium tetrafluoroborate, has been developed. Modifying the FFM originally designed by Liu et al. (J. Phys. Chem. B, 2004, 108, 12978-12989), the electrostatic charges on interacting sites are refined according to partial charges calculated by explicit-ion density functional theory. The refined FFM reproduces experimental heats of vaporization, diffusion coefficients, ionic conductivities, and shear viscosities of RTILs, which is a significant improvement over the original model (Zh. Liu, Sh. Huang and W. Wang, J. Phys. Chem. B, 2004, 108, 12978-12989). The advantages of the proposed procedure include clarity, simplicity, and flexibility. Expanding the functionality of our FFM conveniently only requires modification of the electrostatic charges. Our FFM can be extended to other classes of RTILs as well as condensed matter systems in which the ionic interaction requires an account of polarization effects.
引用
收藏
页码:7910 / 7920
页数:11
相关论文
共 68 条
[1]   Vapourisation of ionic liquids [J].
Armstrong, James P. ;
Hurst, Christopher ;
Jones, Robert G. ;
Licence, Peter ;
Lovelock, Kevin R. J. ;
Satterley, Christopher J. ;
Villar-Garcia, Ignacio J. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2007, 9 (08) :982-990
[2]   DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].
BECKE, AD .
PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100
[3]   Thermodynamic, Dynamic, and Structural Properties of Ionic Liquids Comprised of 1-Butyl-3-methylimidazolium Cation and Nitrate, Azide, or Dicyanamide Anions [J].
Bedrov, Dmitry ;
Borodin, Oleg .
JOURNAL OF PHYSICAL CHEMISTRY B, 2010, 114 (40) :12802-12810
[4]   Influence of Polarization on Structural, Thermodynamic, and Dynamic Properties of Ionic Liquids Obtained from Molecular Dynamics Simulations [J].
Bedrov, Dmitry ;
Borodin, Oleg ;
Li, Zhe ;
Smith, Grant D. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2010, 114 (15) :4984-4997
[5]   Dynamics in a room-temperature ionic liquid: A computer simulation study of 1,3-dimethylimidazolium chloride [J].
Bhargava, BL ;
Balasubramanian, S .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (14)
[6]   Relation between Heat of Vaporization, Ion Transport, Molar Volume, and Cation-Anion Binding Energy for Ionic Liquids [J].
Borodin, Oleg .
JOURNAL OF PHYSICAL CHEMISTRY B, 2009, 113 (36) :12353-12357
[7]   Polarizable Force Field Development and Molecular Dynamics Simulations of Ionic Liquids [J].
Borodin, Oleg .
JOURNAL OF PHYSICAL CHEMISTRY B, 2009, 113 (33) :11463-11478
[8]   Canonical sampling through velocity rescaling [J].
Bussi, Giovanni ;
Donadio, Davide ;
Parrinello, Michele .
JOURNAL OF CHEMICAL PHYSICS, 2007, 126 (01)
[9]   Molecular modeling and experimental studies of the thermodynamic and transport properties of pyridinium-based ionic liquids [J].
Cadena, C ;
Zhao, Q ;
Snurr, RQ ;
Maginn, EJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (06) :2821-2832
[10]   Why is CO2 so soluble in imidazolium-based ionic liquids? [J].
Cadena, C ;
Anthony, JL ;
Shah, JK ;
Morrow, TI ;
Brennecke, JF ;
Maginn, EJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (16) :5300-5308