Concentration-dependent Cycling of Phenothiazine-based Electrolytes in Nonaqueous Redox Flow Cells

Aman Preet Kaur, Bertrand J. Neyhouse, Ilya A. Shkrob, Yilin Wang, N. Harsha Attanayake, Rahul Kant Jha, Qianwen Wu, Lu Zhang, Randy H. Ewoldt, Fikile R. Brushett, Susan A. Odom

Research output: Contribution to journalArticlepeer-review

Abstract

Increasing redox-active species concentrations can improve viability for organic redox flow batteries by enabling higher energy densities, but the required concentrated solutions can become viscous and less conductive, leading to inefficient electrochemical cycling and low material utilization at higher current densities. To better understand these tradeoffs in a model system, we study a highly soluble and stable redox-active couple, N-(2-(2-methoxyethoxy)ethyl)phenothiazine (MEEPT), and its bis(trifluoromethanesulfonyl)imide radical cation salt (MEEPT-TFSI). We measure the physicochemical properties of electrolytes containing 0.2–1 M active species and connect these to symmetric cell cycling behavior, achieving robust cycling performance. Specifically, for a 1 M electrolyte concentration, we demonstrate 94% materials utilization, 89% capacity retention, and 99.8% average coulombic efficiency over 435 h (100 full cycles). This demonstration helps to establish potential for high-performing, concentrated nonaqueous electrolytes and highlights possible failure modes in such systems.

Original languageEnglish
Article numbere202201171
JournalChemistry - An Asian Journal
Volume18
Issue number5
DOIs
StatePublished - Mar 1 2023

Bibliographical note

Funding Information:
This work was supported as part of the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. APK, BJN and FRB gratefully acknowledge partial funding of this work by the National Science Foundation (NSF) under Award Number 1805566. BJN also acknowledges the NSF Graduate Research Fellowship Program under Award Number 2141064. Any opinion, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the NSF. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE‐AC02‐06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid‐up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.

Funding Information:
This work was supported as part of the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. APK, BJN and FRB gratefully acknowledge partial funding of this work by the National Science Foundation (NSF) under Award Number 1805566. BJN also acknowledges the NSF Graduate Research Fellowship Program under Award Number 2141064. Any opinion, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the NSF. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

ASJC Scopus subject areas

  • Biochemistry
  • Organic Chemistry

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