We report viscous flow properties of a redox-active organic molecule, N-(2-(2-methoxyethoxy)ethyl)phenothiazine (MEEPT), a candidate for non-aqueous redox flow batteries, and two of its radical cation salts. A microfluidic viscometer enabled the use of small sample volumes in determining viscosity as a function of shear rate and concentration in the non-aqueous solvent, acetonitrile, both with and without supporting salts. All solutions tested show Newtonian behavior over shear rates of up to 30 000 s−1, which was rationalized by scaling arguments for the diffusion-based relaxation time of a single MEEPT molecule without aggregation. Neat MEEPT is flowable but with a large viscosity (412 at room temperature), which is ∼1000 times larger than that of acetonitrile. MEEPT solutions in acetonitrile have low viscosities; at concentrations up to 0.5 M, the viscosity increases by less than a factor of two. From concentration-dependent viscosity measurements, molecular information was inferred from intrinsic viscosity (hydrodynamic diameter) and the Huggins coefficient (interactions). Model fit credibility was assessed using the Bayesian Information Criterion. It is found that the MEEPT and its charged cations are “flowable” and do not flocculate at concentrations up to 0.5 M. MEEPT has a hydrodynamic diameter of around 8.5 Å, which is almost insensitive to supporting salt and state of charge. This size is comparable to molecular dimensions of single molecules obtained from optimized structures using density functional theory calculations. The results suggest that MEEPT is a promising candidate for redox flow batteries in terms of its viscous flow properties.
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August 2020
Research Article|
August 18 2020
Viscous flow properties and hydrodynamic diameter of phenothiazine-based redox-active molecules in different supporting salt environments
Yilin Wang (王怡琳)
;
Yilin Wang (王怡琳)
1
Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
2
Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
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Aman Preet Kaur
;
Aman Preet Kaur
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
4
Department of Chemistry, University of Kentucky
, Lexington, Kentucky 40506, USA
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N. Harsha Attanayake
;
N. Harsha Attanayake
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
4
Department of Chemistry, University of Kentucky
, Lexington, Kentucky 40506, USA
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Zhou Yu (于洲)
;
Zhou Yu (于洲)
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
5
Materials Science Division, Argonne National Laboratory
, Lemont, Illinois 60439, USA
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Thilini M. Suduwella
;
Thilini M. Suduwella
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
4
Department of Chemistry, University of Kentucky
, Lexington, Kentucky 40506, USA
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Lei Cheng (程蕾)
;
Lei Cheng (程蕾)
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
5
Materials Science Division, Argonne National Laboratory
, Lemont, Illinois 60439, USA
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Susan A. Odom
;
Susan A. Odom
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
4
Department of Chemistry, University of Kentucky
, Lexington, Kentucky 40506, USA
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Randy H. Ewoldt
Randy H. Ewoldt
a)
1
Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
2
Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
6
Materials Research Laboratory, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
a)Author to whom correspondence should be addressed: [email protected]
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Aman Preet Kaur
3,4
N. Harsha Attanayake
3,4
Thilini M. Suduwella
3,4
Susan A. Odom
3,4
Randy H. Ewoldt
1,2,3,6,a)
1
Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
2
Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
3
Joint Center for Energy Storage Research, Argonne National Laboratory
, Lemont, Illinois 60439, USA
4
Department of Chemistry, University of Kentucky
, Lexington, Kentucky 40506, USA
5
Materials Science Division, Argonne National Laboratory
, Lemont, Illinois 60439, USA
6
Materials Research Laboratory, University of Illinois at Urbana-Champaign
, Urbana, Illinois 61801, USA
a)Author to whom correspondence should be addressed: [email protected]
Physics of Fluids 32, 083108 (2020)
Article history
Received:
April 07 2020
Accepted:
July 20 2020
Citation
Yilin Wang, Aman Preet Kaur, N. Harsha Attanayake, Zhou Yu, Thilini M. Suduwella, Lei Cheng, Susan A. Odom, Randy H. Ewoldt; Viscous flow properties and hydrodynamic diameter of phenothiazine-based redox-active molecules in different supporting salt environments. Physics of Fluids 1 August 2020; 32 (8): 083108. https://doi.org/10.1063/5.0010168
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