Preferential solvation of an asymmetric redox molecule

Kee Sung Han; Nav Nidhi Rajput; M. Vijayakumar; Xiaoliang Wei; Wei Wang; Jianzhi Hu; Kristin A. Persson; Karl T. Mueller

doi:10.1021/acs.jpcc.6b09114

Preferential solvation of an asymmetric redox molecule

Kee Sung Han
, Nav Nidhi Rajput
, M. Vijayakumar
, Xiaoliang Wei
, Wei Wang
, Jianzhi Hu
, Kristin A. Persson
, Karl T. Mueller

Materials Science and Engineering

Stony Brook University

Pacific Northwest National Laboratory
Joint Center for Energy Storage Research
Lawrence Berkeley National Laboratory
University of California at Berkeley

Research output: Contribution to journal › Article › peer-review

22 Scopus citations

Abstract

The fundamental correlations between solubility and solvation structure for the electrolyte system comprising N-(ferrocenylmethyl)-N,N-dimethyl-N-ethylammonium bistri-fluoromethylsulfonimide (Fc1N112-TFSI) dissolved in a ternary carbonate solvent mixture is analyzed using combined NMR relaxation and computational methods. Probing the evolution of the solvent-solvent, ion-solvent and ion-ion interactions with an increase in solute concentration provides a molecular level understanding of the solubility limit of the Fc1N112-TFSI system. An increase in solute concentration leads to pronounced Fc1N112-TFSI contact-ion pair formation by diminishing solvent-solvent and ion-solvent type interactions. At the solubility limit, the precipitation of solute is initiated through agglomeration of contaction pairs due to overlapping solvation shells.

Original language	English
Pages (from-to)	27834-27839
Number of pages	6
Journal	Journal of Physical Chemistry C
Volume	120
Issue number	49
DOIs	https://doi.org/10.1021/acs.jpcc.6b09114
State	Published - Dec 15 2016

Access to Document

10.1021/acs.jpcc.6b09114

Cite this

@article{e7621e5c8312453dbf6a4f8beb29428c,

title = "Preferential solvation of an asymmetric redox molecule",

abstract = "The fundamental correlations between solubility and solvation structure for the electrolyte system comprising N-(ferrocenylmethyl)-N,N-dimethyl-N-ethylammonium bistri-fluoromethylsulfonimide (Fc1N112-TFSI) dissolved in a ternary carbonate solvent mixture is analyzed using combined NMR relaxation and computational methods. Probing the evolution of the solvent-solvent, ion-solvent and ion-ion interactions with an increase in solute concentration provides a molecular level understanding of the solubility limit of the Fc1N112-TFSI system. An increase in solute concentration leads to pronounced Fc1N112-TFSI contact-ion pair formation by diminishing solvent-solvent and ion-solvent type interactions. At the solubility limit, the precipitation of solute is initiated through agglomeration of contaction pairs due to overlapping solvation shells.",

author = "Han, \{Kee Sung\} and Rajput, \{Nav Nidhi\} and M. Vijayakumar and Xiaoliang Wei and Wei Wang and Jianzhi Hu and Persson, \{Kristin A.\} and Mueller, \{Karl T.\}",

note = "Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2016",

month = dec,

day = "15",

doi = "10.1021/acs.jpcc.6b09114",

language = "English",

volume = "120",

pages = "27834--27839",

journal = "Journal of Physical Chemistry C",

issn = "1932-7447",

number = "49",

}

TY - JOUR

T1 - Preferential solvation of an asymmetric redox molecule

AU - Han, Kee Sung

AU - Rajput, Nav Nidhi

AU - Vijayakumar, M.

AU - Wei, Xiaoliang

AU - Wang, Wei

AU - Hu, Jianzhi

AU - Persson, Kristin A.

AU - Mueller, Karl T.

PY - 2016/12/15

Y1 - 2016/12/15

N2 - The fundamental correlations between solubility and solvation structure for the electrolyte system comprising N-(ferrocenylmethyl)-N,N-dimethyl-N-ethylammonium bistri-fluoromethylsulfonimide (Fc1N112-TFSI) dissolved in a ternary carbonate solvent mixture is analyzed using combined NMR relaxation and computational methods. Probing the evolution of the solvent-solvent, ion-solvent and ion-ion interactions with an increase in solute concentration provides a molecular level understanding of the solubility limit of the Fc1N112-TFSI system. An increase in solute concentration leads to pronounced Fc1N112-TFSI contact-ion pair formation by diminishing solvent-solvent and ion-solvent type interactions. At the solubility limit, the precipitation of solute is initiated through agglomeration of contaction pairs due to overlapping solvation shells.

AB - The fundamental correlations between solubility and solvation structure for the electrolyte system comprising N-(ferrocenylmethyl)-N,N-dimethyl-N-ethylammonium bistri-fluoromethylsulfonimide (Fc1N112-TFSI) dissolved in a ternary carbonate solvent mixture is analyzed using combined NMR relaxation and computational methods. Probing the evolution of the solvent-solvent, ion-solvent and ion-ion interactions with an increase in solute concentration provides a molecular level understanding of the solubility limit of the Fc1N112-TFSI system. An increase in solute concentration leads to pronounced Fc1N112-TFSI contact-ion pair formation by diminishing solvent-solvent and ion-solvent type interactions. At the solubility limit, the precipitation of solute is initiated through agglomeration of contaction pairs due to overlapping solvation shells.

UR - https://www.scopus.com/pages/publications/85032920068

U2 - 10.1021/acs.jpcc.6b09114

DO - 10.1021/acs.jpcc.6b09114

M3 - Article

SN - 1932-7447

VL - 120

SP - 27834

EP - 27839

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

IS - 49

ER -

Preferential solvation of an asymmetric redox molecule

Abstract

Access to Document

Other files and links

Fingerprint

Cite this